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Time trends and regional differences of polychlorinated dibenzo-p-dioxins and -furans (PCDD/Fs), polychlorinated biphenyls (PCBs), polychlorinated naphthalenes (PCNs), DDTs, polybrominated biphenyls (PBBs) and polybrominated diphenylethers (BDEs) were studied in unhatched osprey eggs collected by bird ringers in 1972-2017 from four areas in Finland. Two study areas were from Baltic Sea, Northern Quark and Finnish Archipelago Sea, while the two others were inland lake areas, eutrophicated Lake Vanajanselkä affected by industrial emissions, and Pristine SW Lake Area. The highest concentrations of most compound groups were in Lake Vanajanselkä consistent with high emissions, the predominance of bream as a prey, and higher concentrations in bream compared to other prey fish. Concentrations of all chlorinated compounds decreased significantly in all study areas. Average annual decreases were ∑PCDD/F 2.3-4.9%, ∑PCB 2.2-4.2%, ∑PCN 2.6-7.0% and ∑DDT 7.1-9.5%, primarily in line with decreased levels in prey fish. From 1972 PBBs and BDEs increased significantly until 1990s declining rapidly thereafter. PCDD/F congener profile was dominated by 2,3,4,7,8-PeCDF, except in Lake Vanajanselkä by 1,2,3,6,7,8-HxCDD. PCB congener profile was dominated by PCB 153 in all study areas, followed by PCB 180 and PCB 138. Among dioxin-like compounds PCBs contributed 82%, PCDDs 14% and PCDFs 4% to toxic equivalent quantity (∑TEQ). PCB 126 contributed most to ∑TEQ, followed by 1,2,3,7,8-PeCDD. BDE 47 being the dominant BDE congener, followed by BDE 100. ∑DDT concentrations were relatively similar across all study areas, with DDE contributing about 90%. Productivity of chicks per active nest was significantly decreased in Lake Vanajanselkä, and the likely explanation is embryotoxicity of dioxin-like compounds. It is plausible that dioxin-like compounds influenced embryonic survival among highly exposed ospreys prior to 2010, especially in Lake Vanajanselkä and Northern Quark. However, decreased survival due to DDE-induced eggshell thinning seems unlikely after 1985, and BDE levels were below those potentially causing adverse effects.

Background: Polychlorinated alkanes (PCAs) constitute a large group of individual congeners originating from commercial chlorinated paraffin (CP) products with carbon chain lengths of PCAs-C10-13, PCAs-C14-17, and PCAs-C18-32, occasionally containing PCAs-C6-9 impurities. The extensive use of CPs has led to global environmental pollution of PCAs. This study aimed to quantify PCAs in paired serum and breast milk of lactating Swedish mothers, exploring their concentration relationship. Methods: Twenty-five paired samples of mothers’ blood serum and breast milk were analysed and concentrations were determined for PCAs C6-32 and compared to 4,4′-DDE, the PCB congener 2,2′,4,4′,5,5′-hexachlorobiphenyl (CB-153), and hexachlorobenzene (HCB). Results: The median concentrations of PCAs-C6-9, PCAs-C10-13, PCAs-C14-17, PCAs-C18-32 and ΣPCAs in serum were 14, 790, 520, 16 and 1350 ng/g lipid weight (lw), respectively, and in breast milk 0.84, 36, 63, 6.0 and 107 ng/g lw. Levels of 4,4′-DDE, CB-153 and HCB were comparable in the two matrices, serum and breast milk at 17, 12 and 4.9 ng/g lw. The results show significant differences of PCAs-C10-13 and PCAs-C14-17 in breast milk with 22– and 6.2-times lower lw-based concentrations than those measured in serum. On wet weight the differences serum/breast milk ratios of PCAs-C6-9, PCAs-C10-13, PCAs-C14-17, PCAs-C18-32 and ΣPCAs were 1.7, 3.2, 1.0, 0.4 and 1.6, respectively, while the ratio for 4,4′-DDE, CB-153 and HCB were each close to 0.1. Conclusion: Swedish lactating mothers had high serum concentrations of PCAs-C10-13 and PCAs-C14-17, with the ΣPCAs median serum concentration of 1350 ng/g lw. The breast milk concentration, although considerably lower at 107 ng/g lw, still surpassed those of 4,4′-DDE, CB-153 and HCB, suggesting an exposure risk of infants to PCAs. The variation in blood and breast milk accumulation between PCAs and studied legacy POPs, is rarely discussed but warrants further studies on partitioning properties as well as associated toxicological implications.

Time trends and regional differences of polychlorinated dibenzo-p-dioxins and -furans (PCDD/Fs), polychlorinated biphenyls (PCBs), polychlorinated naphthalenes (PCNs), DDTs, polybrominated biphenyls (PBBs) and polybrominated diphenylethers (BDEs) were studied in unhatched osprey eggs collected by bird ringers in 1972–2017 from four areas in Finland. Two study areas were from Baltic Sea, Northern Quark and Finnish Archipelago Sea, while the two others were inland lake areas, eutrophicated Lake Vanajanselkä affected by industrial emissions, and Pristine SW Lake Area. The highest concentrations of most compound groups were in Lake Vanajanselkä consistent with high emissions, the predominance of bream as a prey, and higher concentrations in bream compared to other prey fish. Concentrations of all chlorinated compounds decreased significantly in all study areas. Average annual decreases were ∑PCDD/F 2.3–4.9%, ∑PCB 2.2–4.2%, ∑PCN 2.6–7.0% and ∑DDT 7.1–9.5%, primarily in line with decreased levels in prey fish. From 1972 PBBs and BDEs increased significantly until 1990s declining rapidly thereafter. PCDD/F congener profile was dominated by 2,3,4,7,8-PeCDF, except in Lake Vanajanselkä by 1,2,3,6,7,8-HxCDD. PCB congener profile was dominated by PCB 153 in all study areas, followed by PCB 180 and PCB 138. Among dioxin-like compounds PCBs contributed 82%, PCDDs 14% and PCDFs 4% to toxic equivalent quantity (∑TEQ). PCB 126 contributed most to ∑TEQ, followed by 1,2,3,7,8-PeCDD. BDE 47 being the dominant BDE congener, followed by BDE 100. ∑DDT concentrations were relatively similar across all study areas, with DDE contributing about 90%. Productivity of chicks per active nest was significantly decreased in Lake Vanajanselkä, and the likely explanation is embryotoxicity of dioxin-like compounds. It is plausible that dioxin-like compounds influenced embryonic survival among highly exposed ospreys prior to 2010, especially in Lake Vanajanselkä and Northern Quark. However, decreased survival due to DDE-induced eggshell thinning seems unlikely after 1985, and BDE levels were below those potentially causing adverse effects. [ABSTRACT FROM AUTHOR]

Per- and polyfluoroalkyl substances (PFAS) are found ubiquitously in wastewater treatment plants (WWTPs) due to their multiple sources in industry and consumer products. In Australia, limited spatial data are available on PFAS levels in WWTPs influent, while no temporal data have been reported. The aim of this study was to investigate the occurrence and temporal trend of PFAS in the influent of two large WWTPs in Australia (WWTP A and B) over a four-year period. Daily influent samples were collected over one week at different seasons from 2014 to 2017. Eleven perfluoroalkyl acids (PFAA) (i.e. seven perfluoroalkyl carboxylic acids (PFCAs) and four perfluoroalkyl sulfonic acids (PFSA)) were detected with mean Σ11PFAA concentrations of 57 ± 3.3–94 ± 17 ng/L at WWTP A, and 31 ± 6.1–142 ± 73 ng/L at WWTP B. The highest mean concentrations were observed for perfluorohexanoate (PFHxA) (20 ± 2 ng/L) in WWTP A, and perfluorooctane sulfonate (PFOS) (17 ± 13 ng/L) in WWTP B. The precursor 6:2 fluorotelomer sulfonate was detected over five sampling periods from Aug 2016 to Oct 2017, with mean concentrations of 37 ± 18–138 ± 51 ng/L for WWTP A and 8.8 ± 4.5–29 ± 5.1 ng/L for WWTP B. Higher concentration of 6:2 FTS (1.8–11 folds) than those of PFOA and PFOS in WWTP A indicate a likely substitution of C8 PFAA by fluorotelomer-based PFAS in this catchment. Temporal trends (annual and seasonal) in per-capita mass load were observed for some PFAA, increasing for PFPeA, PFHxA, PFHpA, PFNA, and PFHxS, while decreasing for PFBS and PFOS in either WWTPs. Notably, elevated levels of PFOS in October 2017 were observed at both WWTPs with the highest per capita mass load of up to 67 μg/day/inhabitant. For some PFAS release trends, longer sampling periods would be required to achieve acceptable statistical power. Keywords: Per- and polyfluoroalkyl substances (PFAS), 6:2 fluorotelomer sulfonate (6:2 FTS), Temporal trends, Wastewater treatment plant (WWTP), Influent, Power, Effect size

Limited information exists regarding contemporary and historical emissions for many anthropogenic chemicals, especially for contaminants of emerging concern (CECs). This study examined temporal trends of several perfluoroalkyl substances (PFASs), polybrominated diphenyl ethers (PBDEs), and hexabromocyclododecanes (HBCDs) in three beluga whale (Delphinapterus leucas) populations from the Canadian Arctic [Hendrickson Island (HI), NT; Pangnirtung (PG), NU; and Sanikiluaq (SQ), NU] collected from 1982 to 2013. The confounding factors of animal size, age, and sex were included in the analyses, but were only significant for some CECs. The strongest temporal resolution was obtained from HI, which showed increasing trends in PBDEs (4.8%/year) and HBCDs (2.9%/year), and decreases in perfluoroalkylcarboxylic acids (PFCAs, −6.0%/year). Concentrations of perfluorooctanesulfonate (PFOS) were relatively stable between 1984 and 2010, increasing substantially in 2011; trends in perfluorooctanesulfonamide (PFOSA) concentrations were not strictly linear over the study period. PBDE, HBCD, and PFCA trends in the HI population were opposite/different to that of many other arctic animals (e.g., polar bears) for the same time period. Trends were inconsistent among locations, suggesting that regional differences in dietary exposure and/or sources may also impact these trends. The effects of climate-change-driven processes on the exposure and distribution of CECs are currently not well understood, highlighting a need for ongoing contaminant monitoring.

Abstract Background There is a concern that continued emissions of man-made per- and polyfluoroalkyl substances (PFASs) may cause environmental and human health effects. Now widespread in human populations and in the environment, several PFASs are also present in remote regions of the world, but the environmental transport and fate of PFASs are not well understood. Phasing out the manufacture of some types of PFASs started in 2000 and further regulatory and voluntary actions have followed. The objective of this review is to understand the effects of these actions on global scale PFAS concentrations. Methods Searches for primary research studies reporting on temporal variations of PFAS concentrations were performed in bibliographic databases, on the internet, through stakeholder contacts and in review bibliographies. No time, document type, language or geographical constraints were applied in the searches. Relevant subjects included human and environmental samples. Two authors screened all retrieved articles. Dual screening of 10% of the articles was performed at title/abstract and full-text levels by all authors. Kappa tests were used to test consistency. Relevant articles were critically appraised by four reviewers, with double checking of 20% of the articles by a second reviewer. Meta-analysis of included temporal trends was considered but judged to not be appropriate. The trends were therefore discussed in a narrative synthesis. Results Available evidence suggests that human concentrations of perfluorooctane sulfonate (PFOS), perfluorodecane sulfonate (PFDS), and perfluorooctanoic acid (PFOA) generally are declining, while previously increasing concentrations of perfluorohexane sulfonate (PFHxS) have begun to level off. Rapid declines for PFOS-precursors (e.g. perfluorooctane sulfonamide, FOSA) have also been consistently observed in human studies. In contrast, limited data indicate that human concentrations of PFOS and PFOA are increasing in China where the production of these substances has increased. Human concentrations of longer-chained perfluoroalkyl carboxylic acids (PFCAs) with 9–14 carbon atoms are generally increasing or show insignificant trends with too low power to detect a trend. For abiotic and biological environmental samples there are no clear patterns of declining trends. Most substances show mixed results, and a majority of the trends are insignificant with low power to detect a trend. Conclusions For electrochemically derived PFASs, including PFOS and PFOA, most human studies in North America and Europe show consistent statistically significant declines. This contrasts with findings in wildlife and in abiotic environmental samples, suggesting that declining PFOS, PFOS-precursor and PFOA concentrations in humans likely resulted from removal of certain PFASs from commercial products including paper and board used in food packaging. Increasing concentrations of long-chain PFCAs in most matrices, and in most regions, is likely due to increased use of alternative PFASs. Continued temporal trend monitoring in the environment with well-designed studies with high statistical power are necessary to evaluate the effectiveness of past and continuing regulatory mitigation measures. For humans, more temporal trend studies are needed in regions where manufacturing is most intense, as the one human study available in China is much different than in North America or Europe.

Assessing species abundance and reproductive output is crucial for evaluations of population dynamics, conservation status and the development of management objectives. The Caspian seal Pusa caspica is a key predator in the Caspian Sea ecosystem and is listed as Endangered by the IUCN. Here we report on fixed-wing aerial strip transect surveys of the breeding population on the Caspian Sea winter ice field carried out in February, 2005-2012. Potential detection biases were estimated by applying a Petersen mark–recapture estimator to the counts from double photographic observations. We also tested for effects of weather conditions on count results, and for correlations between pup production and ice conditions and net primary productivity (npp). Fluctuations in pup production estimates were observed among years, ranging from 8200 pups (95% CI: 7130-9342) in 2010 to 34000 (95% CI: 31275-36814) in 2005. Total adults on the ice ranged from 14500 in 2010 to 66300 in 2012. We did not detect significant associations between pup production and either ice summary data (ice season length and ice area) or npp. The observed inter-year variation may be partly due to underlying biological drivers influencing the fecundity of the population, although measurement errors arising from observation bias, plus variation in survey timing and weather conditions may also have contributed. Identifying the potential drivers of Caspian seal population dynamics will require extending both the survey time series and the quality of supporting data. However, inter-year fluctuations should still cause concern that the population may be vulnerable to environmental variability and ecosystem dynamics.

Temporal trends of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and dioxin-like polychlorinated biphenyls (DL-PCBs) in mothers' milk are still quite rare. Data are particularly scarce when it comes to concentrations from the last decade, 2000 and onwards. The aims of the present study were to assess temporal trends of PCDD, PCDF and DL-PCB in mothers' milk from Stockholm, 1972–2011 and to compare the results with previous analysis of some of the older samples.The samples were analyzed by high resolution GC/MS and results were statistically evaluated for the periods, 1972–2011 and 2002–2011. The rate of which ∑PCDDs, ∑DL-PCBs and the ∑TEQ are decreasing (on pg/g fat WHO-TEQ2005) is higher in the last decade compared to the 40 year period, 1972–2011. A similar trend is indicated, but not confirmed, for ∑TEQ of PCDFs, probably due to too many PCDF congeners below LOQ in the period 2002–2011. Concentrations of ∑PCDDs, ∑PCDFs, ∑DLPCBs and ∑TEQ, all expressed as pg/g fat on TEQ-WHO2005-basis, show a statistically significant decline over time, 5.8–6.8% per year, 1972–2011. The last ten years the annual declines for ∑PCDDs, ∑DL-PCBs and ∑TEQ are 9.2–11% and for ∑PCDF, 5.4%. Congener specific trend analysis, 2002–2001, of PCDDs and DL-PCBs showed the same pattern, while the PCDF congeners showed no such general trend. The results from the re-analysis showed good agreement with slightly lower ∑TEQ1998 pg/g fat concentrations in six out of seven samples and mean difference of 13% in ∑TEQ1998. The study shows that time series can be elongated from previous studies, as long as the sample population remains the same. Keywords: Mothers' milk, Dioxin, PCDD, PCDF, dioxin-like PCB, Time series

The biliary trematode Pseudamphistomum truncatum parasitizes a wide range of fish-eating mammals, including humans. Here we report the emergence of this parasite in grey seals (Halichoerus grypus) in the Baltic Sea. One hundred eighty-three of 1 554 grey seals (11.9%) examined from 2002-2013 had detectable hepatobiliary trematode infection. Parasite identification was confirmed as P. truncatum by sequencing the ITS2 region of a pool of five to 10 trematodes from each of ten seals collected off the coast of seven different Swedish counties. The proportion of seals parasitized by P. truncatum increased significantly over time and with increasing age of seals. Males were 3.1 times more likely to be parasitized than females and animals killed in fishery interactions were less likely to be parasitized than animals found dead or hunted. There was no significant difference in parasitism of seals examined from the Gulf of Bothnia versus those examined from the Baltic Proper. Although the majority of infections were mild, P. truncatum can cause severe hepatobiliary disease and resulted in liver failure in at least one seal. Because cyprinid fish are the second intermediate host for opisthorchiid trematodes, diets of grey seals from the Baltic Sea were analysed regarding presence of cyprinids. The proportion of gastrointestinal tracts containing cyprinid remains was ten times higher in seals examined from 2008 to 2013 (12.2%) than those examined from 2002 to 2007 (1.2%) and coincided with a general increase of trematode parasitism in the host population. The emergence and relatively common occurrence of P. truncatum in grey seals signals the presence of this parasite in the Baltic Sea ecosystem and demonstrates how aquatic mammals can serve as excellent sentinels of marine ecosystem change. Investigation of drivers behind P. truncatum emergence and infection risk for other mammals, including humans, is highly warranted.

A common and established view is that increased inputs of nutrients to the sea, for example via river flooding, will cause eutrophication and phytoplankton blooms in coastal areas. We here show that this concept may be questioned in certain scenarios. Climate change has been predicted to cause increased inflow of freshwater to coastal areas in northern Europe. River waters in these areas are often brown from the presence of high concentrations of allochthonous dissolved organic carbon (humic carbon), in addition to nitrogen and phosphorus. In this study we investigated whether increased inputs of humic carbon can change the structure and production of the pelagic food web in the recipient seawater. In a mesocosm experiment unfiltered seawater from the northern Baltic Sea was fertilized with inorganic nutrients and humic carbon (CNP), and only with inorganic nutrients (NP). The system responded differently to the humic carbon addition. In NP treatments bacterial, phytoplankton and zooplankton production increased and the systems turned net autotrophic, whereas the CNP-treatment only bacterial and zooplankton production increased driving the system to net heterotrophy. The size-structure of the food web showed large variations in the different treatments. In the enriched NP treatments the phytoplankton community was dominated by filamentous >20 µm algae, while in the CNP treatments the phytoplankton was dominated by picocyanobacteria