Geographical Analysis of Ballast Water Data and Potential Threats of Invasive Species for the North Eastern United States

The globalization of consumer goods and natural resources has led to an unintentional increase in exchanges of native biota (Bright 1999, Barbier and Shogren 2004, Perrings et al. 2005). Organisms that were once constrained to niche native environments are increasingly finding means of transporting themselves to new territories where lack of predation and ideal living conditions allow for geographic takeover. Ballast water discharge and hull fouling have been identified as the main vectors for these introductions (Ruiz et al. 1997, Molnar et al. 2008) which end up causing billions of dollars in economic damage (Pimentel et al. 2005) and invaluable ecological harm (Gurevitch and Padilla 2004)

Temperature and Salinity Tolerances Predict Range Expansion for Two Invasive Marine Invertebrates

Aquatic invasions of nonindigenous species have increased dramatically due to the globalization of consumer goods, which relies on shipping to connect once isolated marine environments (Bright 1999, Barbier and Shogren 2004, Perrings et al. 2005). European waters have been shown to pose a particularly high threat to the northeastern United States due to the disproportionately large amount of shipping arriving from the area (Dassuncao 2008 unpublished) and the presence of invasive species, from regions outside Europe, currently established in European countries (Molnar et al. 2008). One European invader thought to be especially likely to arrive in the near future is the Australasian barnacle, Austrominius (=Elminius) modestus, (J. Pederson, MITSG, 2008), which has a long history in European waters (Crisp 1958, Harms and Anger 1989). Because A. modestus has been present in Europe for over 60 years, the question is why has it not appeared in the U.S? As fouling organisms, barnacles are among those species that are spread readily as invaders

North Atlantic Deep Water formation inhibits high Arctic contamination by continental perfluorooctane sulfonate discharges

Perfluorooctane sulfonate (PFOS) is an aliphatic fluorinated compound with eight carbon atoms that is extremely persistent in the environment and can adversely affect human and ecological health. The stability, low reactivity, and high water solubility of PFOS combined with the North American phase-out in production around the year 2000, make it a potentially useful new tracer for ocean circulation. Here we characterize processes affecting the lifetime and accumulation of PFOS in the North Atlantic Ocean and transport to sensitive Arctic regions by developing a 3-D simulation within the MITgcm. The model captures variability in measurements across biogeographical provinces (R2 = 0.90, p=0.01). In 2015, the North Atlantic PFOS reservoir was equivalent to 60% of cumulative inputs from the North American and European continents (1400 Mg). Cumulative inputs to the Arctic accounted for 30% of continental discharges, while the remaining 10% was transported to the tropical Atlantic and other regions. PFOS concentrations declined rapidly after 2002 in the surface mixed-layer (half-life: 1-2 years) but are still increasing below 1000 m depth. During peak production years (1980-2000), plumes of PFOS enriched seawater were transported to the Subarctic in energetic surface ocean currents. However, Atlantic Meridional Overturning Circulation (AMOC) and deep ocean transport returned a substantial fraction of this northward transport (20%, 530 Mg) to southern latitudes and reduced cumulative inputs to the Arctic (730 Mg) by 70%. Weakened AMOC due to climate change is thus likely to increase the magnitude of persistent bioaccumulative pollutants entering the Arctic Ocean

Vertical Profiles, Sources and Transport of PFASs in the Arctic Ocean

The relative importance of atmospheric versus oceanic transport for poly- and perfluorinated alkyl substances (PFASs) reaching the Arctic Ocean is not well understood. Vertical profiles from the Central Arctic Ocean and shelf water, snow and meltwater samples were collected in 2012; 13 PFASs (C6-C12 PFCAs; C6, 8, 10 PFSAs; MeFOSAA and EtFOSAA, and FOSA) were routinely detected (range: \u3c5 – 343 pg/L). PFASs were only detectable above 150 m depth in the polar mixed layer (PML) and halocline. Enhanced concentrations were observed in snow and meltpond samples, implying atmospheric deposition as an important source of PFASs. Model results suggested atmospheric inputs to account for 34-59% (~11-19 pg/L) of PFASs. Model results suggested atmospheric inputs to account for 34-59% (~11-19 pg/L) of measured PFOA concentrations in the PML (mean 32±15 pg/L). Modeled surface and halocline measurements for PFOS based on North Atlantic inflow (11-36 pg/L) agreed with measurements (mean, 17, range \u3c5-41 pg/L). Modeled deep water concentrations below 200 m (5-15 pg/L) were slightly higher than measurements (\u3c5 pg/L), suggesting the lower bound of PFAS emissions estimates from wastewater and rivers may provide the best estimate of inputs to the Arctic. Despite low concentrations in deep water, this reservoir is expected to contain most of the PFOS mass in the Arctic (63-180 Mg) and projected to continue increasing to 2038

Source attribution of poly- and perfluoroalkyl substances (PFASs) in surface waters from Rhode Island and the New York Metropolitan Area

Exposure to poly- and perfluoroalkyl substances (PFASs) has been associated with adverse health effects in humans and wildlife. Understanding pollution sources is essential for environmental regulation, but source attribution for PFASs has been confounded by limited information about industrial releases and rapid changes in chemical production. Here we use principal component analysis (PCA), hierarchical clustering, and geospatial analysis to understand source contributions to 14 PFASs measured across 37 sites in the northeastern United States in 2014. PFASs are significantly elevated in urban areas compared to rural sites except for perfluorobutanesulfonate, N-methyl perfluorooctanesulfonamidoacetic acid, perfluoroundecanate, and perfluorododecanate. The highest PFAS concentrations across sites were those of perfluorooctanate (PFOA, 56 ng L−1) and perfluorohexanesulfonate (PFHxS, 43 ng L−1), and perfluorooctanesulfonate (PFOS) levels are lower than earlier measurements of U.S. surface waters. PCA and cluster analysis indicate three main statistical groupings of PFASs. Geospatial analysis of watersheds reveals the first component/cluster originates from a mixture of contemporary point sources such as airports and textile mills. Atmospheric sources from the waste sector are consistent with the second component, and the metal smelting industry plausibly explains the third component. We find this source-attribution technique is effective for better understanding PFAS sources in urban areas

PFAS and Precursor Bioaccumulation in Freshwater Recreational Fish: Implications for Fish Advisories

Per- and polyfluoroalkyl substances (PFAS) are a diverse class of fluorinated anthropogenic chemicals that include perfluoroalkyl acids (PFAA), which are widely used in modern commerce. Many products and environmental samples contain abundant precursors that can degrade into terminal PFAA associated with adverse health effects. Fish consumption is an important dietary exposure source for PFAS that bioaccumulate in food webs. However, little is known about bioaccumulation of PFAA precursors. Here, we identify and quantify PFAS in recreational fish species collected from surface waters across New Hampshire, US, using a toolbox of analytical methods. Targeted analysis of paired water and tissue samples suggests that many precursors below detection in water have a higher bioaccumulation potential than their terminal PFAA. Perfluorobutane sulfonamide (FBSA), a short-chain precursor produced by electrochemical fluorination, was detected in all fish samples analyzed for this compound. The total oxidizable precursor assay interpreted using Bayesian inference revealed fish muscle tissue contained additional, short-chain precursors in high concentration samples. Suspect screening analysis indicated these were perfluoroalkyl sulfonamide precursors with three and five perfluorinated carbons. Fish consumption advisories are primarily being developed for perfluorooctane sulfonate (PFOS), but this work reinforces the need for risk evaluations to consider additional bioaccumulative PFAS, including perfluoroalkyl sulfonamide precursors

Source Attribution of Poly- and Perfluoroalkyl Substances (PFASs) in Surface Waters from Rhode Island and the New York Metropolitan Area

Exposure to poly- and perfluoroalkyl substances (PFASs) has been associated with adverse health effects in humans and wildlife. Understanding pollution sources is essential for environmental regulation, but source attribution for PFASs has been confounded by limited information about industrial releases and rapid changes in chemical production. Here we use principal component analysis (PCA), hierarchical clustering, and geospatial analysis to understand source contributions to 14 PFASs measured across 37 sites in the northeastern United States in 2014. PFASs are significantly elevated in urban areas compared to rural sites except for perfluorobutanesulfonate, N-methyl perfluorooctanesulfonamidoacetic acid, perfluoroundecanate, and perfluorododecanate. The highest PFAS concentrations across sites were those of perfluorooctanate (PFOA, 56 ng L−1) and perfluorohexanesulfonate (PFHxS, 43 ng L−1), and perfluorooctanesulfonate (PFOS) levels are lower than earlier measurements of U.S. surface waters. PCA and cluster analysis indicate three main statistical groupings of PFASs. Geospatial analysis of watersheds reveals the first component/cluster originates from a mixture of contemporary point sources such as airports and textile mills. Atmospheric sources from the waste sector are consistent with the second component, and the metal smelting industry plausibly explains the third component. We find this source-attribution technique is effective for better understanding PFAS sources in urban areas.Engineering and Applied Science

A Model for Methylmercury Uptake and Trophic Transfer by Marine Plankton

Methylmercury (MeHg) concentrations can increase by 100 000 times between seawater and marine phytoplankton, but levels vary across sites. To better understand how ecosystem properties affect variability in planktonic MeHg concentrations, we develop a model for MeHg uptake and trophic transfer at the base of marine food webs. The model successfully reproduces measured concentrations in phytoplankton and zooplankton across diverse sites from the Northwest Atlantic Ocean. Highest MeHg concentrations in phytoplankton are simulated under low dissolved organic carbon (DOC) concentrations and ultraoligotrophic conditions typical of open ocean regions. This occurs because large organic complexes bound to MeHg inhibit cellular uptake and cell surface area to volume ratios are greatest under low productivity conditions. Modeled bioaccumulation factors for phytoplankton (102.4–105.9) are more variable than those for zooplankton (104.6–106.2) across ranges in DOC (40–500 μM) and productivities (ultraoligotrophic to hypereutrophic) typically found in marine ecosystems. Zooplankton growth dilutes their MeHg body burden, but they also consume greater quantities of MeHg enriched prey at larger sizes. These competing processes lead to lower variability in MeHg concentrations in zooplankton compared to phytoplankton. Even under hypereutrophic conditions, modeled growth dilution in marine zooplankton is insufficient to lower their MeHg concentrations, contrasting findings from freshwater ecosystems

Can profiles of poly- and Perfluoroalkyl substances (PFASs) in human serum provide information on major exposure sources?

Background: Humans are exposed to poly- and perfluoroalkyl substances (PFASs) from diverse sources and this has been associated with negative health impacts. Advances in analytical methods have enabled routine detection of more than 15 PFASs in human sera, allowing better profiling of PFAS exposures. The composition of PFASs in human sera reflects the complexity of exposure sources but source identification can be confounded by differences in toxicokinetics affecting uptake, distribution, and elimination. Common PFASs, such as perfluorooctanoic acid (PFOA), perfluorooctane sulfonic acid (PFOS) and their precursors are ubiquitous in multiple exposure sources. However, their composition varies among sources, which may impact associated adverse health effects. Methods: We use available PFAS concentrations from several demographic groups in a North Atlantic seafood consuming population (Faroe Islands) to explore whether chemical fingerprints in human sera provide insights into predominant exposure sources. We compare serum PFAS profiles from Faroese individuals to other North American populations to investigate commonalities in potential exposure sources. We compare individuals with similar demographic and physiological characteristics and samples from the same years to reduce confounding by toxicokinetic differences and changing environmental releases. Results: Using principal components analysis (PCA) confirmed by hierarchical clustering, we assess variability in serum PFAS concentrations across three Faroese groups. The first principal component (PC)/cluster consists of C9-C12 perfluoroalkyl carboxylates (PFCAs) and is consistent with measured PFAS profiles in consumed seafood. The second PC/cluster includes perfluorohexanesulfonic acid (PFHxS) and the PFOS precursor N-ethyl perfluorooctane sulfonamidoacetate (N-EtFOSAA), which are directly used or metabolized from fluorochemicals in consumer products such as carpet and food packaging. We find that the same compounds are associated with the same exposure sources in two North American populations, suggesting generalizability of results from the Faroese population. Conclusions: We conclude that PFAS homologue profiles in serum provide valuable information on major exposure sources. It is essential to compare samples collected at similar time periods and to correct for demographic groups that are highly affected by differences in physiological processes (e.g., pregnancy). Information on PFAS homologue profiles is crucial for attributing adverse health effects to the proper mixtures or individual PFASs. Electronic supplementary material The online version of this article (10.1186/s12940-018-0355-4) contains supplementary material, which is available to authorized users