Organohalogen Contaminants Research Articles

Influence of paternal factors on plastic ingestion and brominated chemical exposure in East Tropical Atlantic Procellariid chicks

The presence of plastic debris and organo-brominated compounds in the marine environment poses a concern to wildlife. Plastic can absorb and release chemical compounds, making their ingestion potentially harmful, while chemical compounds have become omnipresent, with a tendency to bioaccumulate in the food web. Seabirds are often used as indicators of marine plastic pollution, yet studies on the exposure of tropical communities to plastic contamination are still scarce. In this study we monitored the amounts of plastics in faeces and organo-brominated compounds ingested/assimilated in feathers by adults and chicks of Cape Verde shearwaters and Bulwer's petrels from Cabo Verde. Anthropogenic pollutants, polybrominated diphenyl ethers (PBDEs), and naturally generated methoxylated-PBDEs (MeO-PBDEs) were among the probed compounds. The frequency of plastic debris ingestion was similar in both species' adults and chicks, although, the characteristics of the ingested plastic differed. Frequency and number of microplastics increased throughout the nestling season for chicks from both species. All species and age groups showed the presence of PBDEs and MeO-PBDEs. Among PBDEs, Bulwer's petrels exhibited higher concentrations than Cape Verde shearwaters, and chicks had higher concentration profiles than adults. Specifically, Bulwer's petrel chicks showed higher concentrations than Cape Verde shearwater chicks. On the contrary, Cape Verde shearwater adults exhibited higher occurrence and concentrations of MeO-PBDEs when compared to Cape Verde shearwater chicks. We found no effect of plastic loadings or loadings of organohalogen contaminants on body condition or size, although harmful effects may be hidden or reveal themselves in a medium- to long-term. Feather samples from both adults and chicks were shown to be useful for comparing intraspecific contamination levels and appear suitable for the long-term assessment of organohalogen contaminants in seabirds. Species-specific foraging and feeding strategies are likely the drivers of the observed variation in organochlorine contamination burdens among seabird species.

Variations in thyroid hormone levels in endangered St. Lawrence Estuary belugas: Potential linkage with stress and organohalogen contaminant exposure

The St. Lawrence Estuary (SLE) beluga (Delphinapterus leucas) population is highly exposed to an array of contaminants that were identified as one of the causes to the non-recovery of this endangered and declining population. In the last decade, an increasing number of parturition-associated complications and calf mortality has been reported in this population. It was suggested that elevated exposure to organohalogens (e.g., the halogenated flame retardants polybrominated diphenyl ethers [PBDEs]) and stress could play a role in this phenomenon by perturbing thyroid hormones. The objective of this study was to investigate the impact of concentrations of organohalogen contaminants and stress (cortisol levels) on thyroid hormone variations in adult male and female SLE belugas. Because plasma could not be collected in SLE belugas for ethical reasons, skin biopsy (n = 40) was used as a less-invasive alternative matrix to determine organohalogens (PBDEs and other halogenated flame retardants, polychlorinated biphenyls, and organochlorine pesticides), cortisol, and thyroid hormones (triiodothyronine [T3] and thyroxine [T4]), and their metabolites reverse T3 and 3,5-diiodothyronine [3,5-T2]). Cortisol and thyroid hormones were analyzed by ultra-performance liquid chromatography-multiple reactions monitoring mass spectrometry (UPLC-MRM/MS). This method was compared using skin and plasma samples obtained from Arctic belugas. Comparisons of linear models showed that cortisol was a weak predictor for T4, rT3 and 3,5-T2. Specifically, there was a weak significant negative association between T4 and cortisol levels. Moreover, in male SLE belugas, a weak significant positive association was found between T3 and Σ34PBDE concentrations in skin. Our findings suggest that stress (i.e., elevated skin cortisol levels) along with organohalogen exposure (mainly PBDEs) may be associated with thyroid hormone level perturbations in skin of cetaceans.

Organohalogen contaminants threaten the survival of indo-pacific humpback dolphin calves in their largest habitat

As long-lived apex predators, marine mammal adults often accumulate alarmingly levels of environmental contaminants. Nevertheless, the accumulation and risks of these contaminants in the critical calf stage of marine mammals remain largely unknown. Here, we investigated the exposure status and health risks of 74 organohalogen contaminants (OHCs) in Indo-Pacific humpback dolphin calves (Sousa chinensis) collected from the Pearl River Estuary (PRE), China, during 2005–2019. Our findings revealed moderate levels of polychlorinated biphenyls (PCBs), medium-high levels of dichlorodiphenyltrichloroethanes (DDTs) and hexachlorocyclohexanes (HCHs), and the highest levels of polybrominated diphenyl ethers (PBDEs) and alternative halogenated flame retardants (AHFRs) compared to those reported for cetaceans elsewhere. Traditional OHCs like DDTs, PCBs, and PBDEs did not exhibit significant decreasing trends in the dolphin calves despite global restrictions on these compounds, and AHFRs as emerging OHCs showed an increasing trend over the study period. Risk quotients of DDTs, HCHs, PBDEs, and PCBs in most of the dolphin samples were > 1, indicating that humpback dolphin calves may have suffered long-term threats from OHC exposure. The significant correlation observed between the traditional OHC levels and the stranding death number of the dolphin calves suggests these OHCs may impact the survival of this endangered species.

Emerging investigator series: nontargeted screening of aryl hydrocarbon receptor agonists in endangered beluga whales from the St. Lawrence Estuary: beyond legacy contaminants.

The elevated concentrations of organohalogen contaminants in the endangered St. Lawrence Estuary (SLE) belugas have prompted the hypothesis that aryl hydrocarbon receptor (AhR) activity may be a contributor towards their potential adverse effects. While indirect associations between AhR and contaminant levels have been reported in SLE beluga tissues, AhR activity was never directly measured. Using bioassays and nontargeted analysis, this study contrasted AhR activity and agonist profiles between pooled tissue extracts of endangered SLE and non-threatened Arctic belugas. Tissue extracts of SLE belugas exhibited significantly higher overall AhR activity than that of Arctic belugas, with a 2000s SLE beluga liver extract exerting significantly higher activity than blubber extracts of SLE and Arctic belugas from the same time period. Contrary to our expectations, well-known AhR agonists detected by nontargeted analysis, including polychlorinated biphenyls (PCBs), were only minor contributors to the observed AhR activity. Instead, Tox21 suspect screening identified more polar chemicals, such as dyes and natural indoles, as potential contributors. Notably, the natural product bromoindole was selectively detected in SLE beluga liver at high abundance and was further confirmed as an AhR agonist. These findings highlighted the significance of the AhR-mediated toxicity pathway in belugas and underscored the importance of novel AhR agonists, particularly polar compounds, in its induction.

Multi-level assessment of the origin, feeding area and organohalogen contamination on salmon from the Baltic Sea

The Atlantic salmon (Salmo salar) population in the Baltic Sea consists of wild and hatchery-reared fish that have been released into the sea to support salmon stocks. During feeding migration, salmon migrate to different parts of the Baltic Sea and are exposed to various biotic and abiotic stressors, such as organohalogen compounds (OHCs). The effects of salmon origin (wild or hatchery-reared), feeding area (Baltic Main Basin, Bothnian Sea, and Gulf of Finland), and OHC concentration on the differences in hepatic proteome of salmon were investigated. Multi-level analysis of the OHC concentration, transcriptome, proteome, and oxidative stress biomarkers measured from the same salmon individuals were performed to find the key variables (origin, feeding area, OHC concentrations, and oxidative stress) that best account for the differences in the transcriptome and proteome between the salmon groups. When comparing wild and hatchery-reared salmon, differences were found in xenobiotic and amino acid metabolism-related pathways. When comparing salmon from different feeding areas, the amino acid and carbohydrate metabolic pathways were notably different. Several proteins found in these pathways are correlated with the concentrations of polychlorinated biphenyls (PCBs). The multi-level analysis also revealed amino acid metabolic pathways in connection with PCBs and oxidative stress variables related to glutathione metabolism. Other pathways found in the multi-level analysis included genetic information processes related to ribosomes, signaling and cellular processes related to the cytoskeleton, and the immune system, which were connected mainly to the concentrations of Polychlorinated biphenyls and Dichlorodiphenyltrichloroethane and their metabolites. These results suggest that the hepatic proteome of salmon in the Baltic Sea, together with the transcriptome, is more affected by the OHC concentrations and oxidative stress of the feeding area than the origin of the salmon.

Fatty acids and organohalogen contaminants in seafood from the Pearl River Estuary, China: Risk-benefit analyses of seafood consumption

Seafood has long been considered a healthy food choice, but it is also an exposure source of contaminants that may bring potential health risks to humans. Here, 80 organohalogen contaminants (OHCs) and 36 fatty acids (FAs) were analyzed in 22 (n = 211) and 19 fishery species (n = 176) from the eastern- and western Pearl River Estuary (PRE), respectively, for risk–benefit analysis. The average concentrations of total FAs in seafood from the eastern- and western PRE were 26.0 ± 2.14 and 21.3 ± 1.66 mg g−1 wet weight, respectively. Seafood from the eastern PRE exhibited higher levels of OHCs than those from the western PRE, highlighting the spatial heterogeneity of OHC contamination within the PRE. Species occupying higher trophic levels (TLs) typically demonstrated higher levels of OHC accumulation, indicating the biomagnification potential of these contaminants in the PRE ecosystem. Significant negative correlations were observed between TLs and the proportions of monounsaturated fatty acids and polyunsaturated fatty acids, presumably attributed to the ability of fish to synthesize these FAs decreases with increasing TLs. Our benefit-risk quotient (BRQ) analyses revealed that, as far as OHCs are concerned, all seafood species had a BRQ∑OHCs value <1, except for one-spot snapper and daggertooth pike conger, which had BRQ values of 1.03 and 1.14, respectively. The findings indicate that most marine species here analyzed may not pose significant health risks to consumers as a result of OHC exposure. However, considering that many other pollutants and nutrients are not analyzed here, the results of our risk assessments should be treated as preliminary, not final. Future data collection is essential to enhance the comprehensiveness of this type of analysis.

Fatty acids as bioindicators of organohalogen exposure in marine fish from a highly polluted estuary: First insight into small-scale regional differences

Increasing evidence has revealed the lipid-disrupting effects of organic contaminants on aquatic organisms, raising attention about the efficacy of fatty acids (FAs) as bioindicator of contaminant exposure on marine organisms. Here, we investigated the concentrations of 55 organohalogen contaminants (OHCs), 35 FAs, and their correlations in 15 marine fish species (n = 274) from the estuary outlets of the west four region (WFR) and Lingdingyang (LDY) waters in the Pearl River Estuary (PRE), respectively. Despite the similar OHC profiles, significantly higher concentrations of ∑55OHCs were detected in fish from the LDY than those in the WFR. However, FAs in the LDY fish generally contained lower proportions of polyunsaturated fatty acids than in the WFR fish. A total of 148 and 221 significant correlations between OHCs and FAs were observed in fish samples from the LDY and WFR, respectively, supporting that FAs could be efficient bioindicators of OHC stress in marine fish. However, the low overlaps (14/369) of OHC-FA correlations in fish from the two regions suggested that the bioindicators of OHCs might have spatial heterogeneity. Our results highlighted that FAs likely act as potential bioindicators of OHCs in marine fish, while the regional-specific characteristic of the bioindicators should be considered.

Multi-Level Effect Assessment of the Origin, Feeding Area and Organohalogen Contamination on Salmon from the Baltic Sea

Multi-Level Effect Assessment of the Origin, Feeding Area and Organohalogen Contamination on Salmon from the Baltic Sea

A large diversity of organohalogen contaminants reach the meso- and bathypelagic organisms in the Bay of Biscay (northeast Atlantic).

Deep-sea ecosystems play a key role in the cycling and vertical transfer of matter and energy in oceans. Although the contamination of deep-sea demersal and benthic organisms by persistent organic pollutants has been proven, deep pelagic species have been far less studied. To fill these gaps, we studied the occurrence of a large variety of hydrophobic organic contaminants including polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), legacy and alternative brominated flame retardants (BFRs) and per- and polyfluoroalkyl substances (PFASs) in crustaceans and fish species collected in the Bay of Biscay, northeast Atlantic. The results highlighted the global predominance of PCBs in fish, followed by OCPs, PFASs and PBDEs, with highly variable concentrations among species. Most of the chlorinated or brominated contaminants showed increasing concentrations with increasing δ15N values, while most PFASs showed inverse trends. The contaminant profiles and diagnostic ratios revealed species-specific metabolic capacities and peculiar contribution of highly-brominated BFRs.

Teratogenic Effects of Organohalogen Contaminants Extracted from Whale Bacon in a Whole-Rat-Embryo Culture System.

Marine foods can be contaminated with organochlorines and the risk to human beings who consume these foods needs to be evaluated. We examined the teratogenic effects of contaminants extracted from whale bacon on rat embryos using a whole-embryo culture system. Embryonic day 11.5 embryos were cultured for 48 h with organohalogens extracted from whale bacon at low (polychlorinated biphenyls (PCBs): 0.32 ppm, dichlorodiphenyltrichloroethanes (DDTs): 0.16 ppm, chlordanes (CHLs): 0.02 ppm) and high (PCBs: 2.15 ppm, DDTs: 1.99 ppm, CHLs: 0.20 ppm) doses. The levels of organohalogen compounds in cultured embryos were determined. The organochlorine contaminants extracted from whale products were readily transferred to the cultured rat embryos. The number of heartbeats, yolk sac circulation score, and embryonic body circulation score of embryos did not change during the culture period in either exposure group. Cultured embryos treated with the low-dose contaminated medium for 48 h showed abnormalities of the mandible, and craniofacial or forelimb hematomas with an incidence of 50%. All embryos treated with the high-dose medium showed craniofacial abnormalities and cleft lip, and limb abnormalities and hematomas. These results indicate that the organohalogen contaminants in whale bacon may be teratogenic in a dose-dependent manner. Further studies are necessary to determine the dose–effect relationship.

Health impact assessment of pet cats caused by organohalogen contaminants by serum metabolomics and thyroid hormone analysis

Companion animals are in close contact with the human surroundings, and there is growing concern about the effects of harmful substances on the health of pet cats. In this study, we investigated the potential health effects of organohalogen compounds (OHCs) on thyroid hormone (TH) homeostasis and metabolomics in Japanese pet cats. There was a significant negative correlation between concentrations of several contaminants, such as polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), hydroxylated PCBs (OH-PCBs), hydroxylated PBDEs (OH-PBDEs), and THs in cat serum samples. These results suggested that exposure to OHCs causes a decrease in serum TH levels in pet cats.In this metabolomics study, each exposure level of parent compounds (PCBs and PBDEs) and their hydroxylated compounds (OH-PCBs and OH-PBDEs) were associated with their own unique primary metabolic pathways, suggesting that parent and phenolic compounds exhibit different mechanisms of action and biological effects. PCBs were associated with many metabolic pathways, including glutathione and purine metabolism, and the effects were replicated in in-vivo cat PCB administration studies. These results demonstrated that OHC exposure causes chronic oxidative stress in pet cats. PBDEs were positively associated with alanine, aspartate, and glutamate metabolism. Due to the chronic exposure of cats to mixtures of these contaminants, the combination of their respective metabolic pathways may have a synergistic effect.

Ecosystem specific accumulation of organohalogenated compounds: A comparison between adjacent freshwater and terrestrial avian predators

Insight into processes determining the exposure of organohalogenated contaminants (OHCs) in wildlife might be gained from comparing predators in different ecosystems. This study compared two avian predator species with similar food chain lengths: the goldeneye duck (Bucephala clangula) and the tawny owl (Strix aluco) breeding in adjacent freshwater- and terrestrial ecosystems in central Norway. We measured lipophilic organochlorines (OCs) and protein-bound perfluorinated substances (PFASs) in eggs of the two species over 21 years (1999–2019). Across years, the proportional distribution of OCs (∼90% of the ΣOHC load) relative to PFASs (∼10%) was similar in the two species. Moreover, ΣOC concentrations were similar between the species, but PFAS compounds were 2–12 times higher in the goldeneyes than in tawny owls. OC-pesticides dominated in tawny owls (∼60% of ΣOC), whereas persistent polychlorinated biphenyl (PCBs) congeners were the main OC components in goldeneyes (∼70% of ΣOC). The lipid-normalized concentrations of most OC-pesticides and the less persistent PCB101 declined significantly in both species. Hexachlorobenzene (HCB), p,p’-dichlorodiphenyldichloroethylene (p,p’-DDE), and more persistent PCBs decreased in tawny owls, while they tended to increase in goldeneyes. The increase in HCB was particulary robust. Among the PFASs, contrasted temporal trends were found across the species for four out of 11 compounds: PFOS declined while most perfluorocarboxylic acids (PFCAs) increased in tawny owls. In contrast, most PFASs were stable in goldeneyes. Moreover, there was no annual covariance between the OHC exposure in the two species: i.e., high concentrations in one species in a given year did not translate into high concentrations in the other. Hence, the two avian predators in adjacent ecosystems seem to be subject to different processes determining the OHC exposure, probably related to variation in diet and climate, long-range transport of different contaminants, and emissions of pollution locally.

Feathers as an integrated measure of organohalogen contamination, its dietary sources and corticosterone in nestlings of a terrestrial bird of prey, the northern Goshawk (Accipiter gentilis)

In this study, we evaluated the suitability of body feathers, preen oil and plasma for estimation of organohalogen compound (OHC) exposure in northern goshawk Accipiter gentilis nestlings (n = 37; 14 nests). In addition, body feathers received further examination concerning their potential to provide an integrated assessment of (1) OHC exposure, (2) its dietary sources (carbon sources and trophic position) and (3) adrenal gland response (corticosterone). While tetrabromobisphenol A was not detected in any sample, the presence of polychlorinated biphenyls, organochlorine pesticides, polybrominated diphenyl ethers and hexabromocyclododecane in body feathers (median: 23, 19, 1.6 and 3.5 ng g−1 respectively), plasma (median: 7.5, 6.2, 0.50 and 1.0 ng g−1 ww, respectively) and preen oil (median: 750, 600, 18 and 9.57 ng g−1 ww, respectively) suggests analytical suitability for biomonitoring of major OHCs in the three matrices. Furthermore, strong and significant associations (0.20 ≤ R2 ≤ 0.98; all P < 0.05) among the OHC concentrations in all three tissues showed that body feathers and preen oil reliably reflect circulating plasma OHC levels. Of the dietary proxies, δ13C (carbon source) was the most suitable predictor for variation in feather OHCs concentrations, while no significant relationships between body feather OHCs and δ15N (trophic position) were found. Finally, body feather corticosterone concentrations were not related to variation in OHC concentrations. This is the first study to evaluate feathers of a terrestrial bird of prey as an integrated non-destructive tool to jointly assess nestling ecophysiology and ecotoxicology.

A Large Diversity of Organohalogen Contaminants Reach the Meso- and Bathypelagic Organisms in the Bay of Biscay (Northeast Atlantic)

A Large Diversity of Organohalogen Contaminants Reach the Meso- and Bathypelagic Organisms in the Bay of Biscay (Northeast Atlantic)

Within and between breeding-season changes in contaminant occurrence and body condition in the Antarctic breeding south polar skua

The Antarctic ecosystem represents a remote region far from point sources of pollution. Still, Antarctic marine predators, such as seabirds, are exposed to organohalogen contaminants (OHCs) which may induce adverse health effects. With increasing restrictions and regulations on OHCs, the levels and exposure are expected to decrease over time. We studied south polar skua (Catharacta maccormiciki), a top predator seabird, to compare OHC concentrations measured in whole blood from 2001/2002 and 2013/2014 in Dronning Maud Land. As a previous study found increasing organochlorine concentrations with sampling day during the 2001/2002 breeding season, suggesting dietary changes, we investigated if this increase was repeated in the 2013/2014 breeding season. In addition to organochlorines, we analyzed hydroxy-metabolites, brominated contaminants and per- and polyfluoroalkyl substances (PFAS) in 2013/2014, as well as dietary descriptors of stable isotopes of carbon and nitrogen, to assess potential changes in diet during breeding. Lipid normalized concentrations of individual OHCs were 63%, 87% and 105% higher for hexachlorobenzene (HCB), 1,1-dichloro-2,2-bis (p-chlorophenyl)ethylene (p,p'-DDE), and ∑Polychlorinated biphenyls (PCBs), respectively, in 2013/2014 compared to 2001/2002. South polar skuas males in 2013/2014 were in poorer body condition than in 2001/2002, and with higher pollutant levels. Poorer body condition may cause the remobilization of contaminants from stored body reserves, and continued exposure to legacy contaminants at overwintering areas may explain the unexpected higher OHC concentrations in 2013/2014 than 2001/2002. Concentrations of protein-associated PFAS increased with sampling day during the 2013/2014 breeding season, whereas the lipid-soluble chlorinated pesticides, PCBs and polybrominated diphenyl ether (PBDEs) showed no change. OHC occurrence was not correlated with stable isotopes. The PFAS biomagnification through the local food web at the colony should be investigated further.

Seasonal rainfall affects occurrence of organohalogen contaminants in tropical marine fishes and prawns from Zanzibar, Tanzania

Seasonal differences in precipitation may affect contaminant dynamics in tropical coastal regions due to terrestrial runoff of contaminants to the marine environment after the rainy seasons. To assess the effect of seasonal rainfall on occurrence of organohalogen contaminants in a coastal ecosystem, marine fishes and prawns were collected off the coast of Zanzibar, Tanzania in January and August 2018, representing pre- and post-rainy season, respectively. Samples were analyzed for organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs), brominated flame retardants (BFRs), including polybrominated diphenyl ethers (PBDEs) and emerging BFRs, as well as the dietary descriptors stable isotopes of carbon (δ13C) and nitrogen (δ15N). Across all species and seasons, mean contaminant concentrations ranged from below limit of detection (LOD) to 129 ng/g lipid weight (lw) ΣPCBs; 5.6–336 ng/g lw ΣOCPs; and < LOD –22.1 ng/g lw ΣPBDEs. Most of the emerging BFRs were below LOD. Contaminant concentrations generally increased with higher pelagic carbon signal (δ13C) and higher relative trophic position (δ15N). The ratio of DDE/ΣDDTs in fishes and prawns was lower in August than in January, suggesting runoff of non-degraded DDT into the marine system during or after the seasonal rainfall. Contaminant patterns of OCPs and PCBs, and concentrations of BFRs, differed between seasons in all species. A higher relative concentration-increase in lower halogenated, more mobile PCB and PBDE congeners, compared to higher halogenated congeners with lower mobility, between January and August aligns with a signal and effect of terrestrial runoff following the rainy season.

Extractable organochlorine (EOCl) and extractable organobromine (EOBr) in GPC-fractionated extracts from high-trophic-level mammals: Species-specific profiles and contributions of legacy organohalogen contaminants

Previous studies have suggested that unidentified compounds constitute a large proportion of extractable organochlorine (EOCl) and extractable organobromine (EOBr) in the crude extracts without fractionation; however, the proportion of unidentified EOX (X = chlorine, bromine) associated with high-/low-molecular-weight compounds is still unknown. In this study, we applied gel permeation chromatography to fractionate extracts from archived liver samples of high-trophic marine and terrestrial mammals (striped dolphins, cats, and raccoon dogs), for which concentrations of legacy organohalogen contaminants (polychlorinated biphenyls, organochlorine pesticides, and polybrominated diphenyl ethers [PBDEs]) had been previously reported. EOX in high- (>1000 g/mol) and low- (≤1000 g/mol) molecular-weight fractions (EOX-H and EOX-L) were determined by neutron activation analysis. Comparison of EOCl and EOBr enabled the characterization among species. Despite small differences in the concentrations and molecular-weight profiles of EOCl among species, the contribution of chlorine in identified compounds to EOCl-L varied from 1.5% (cats) to 79% (striped dolphins). Considerable species-specific variations were observed in the concentrations of EOBr: striped dolphins exhibited significantly greater concentrations of both EOBr-H and EOBr-L than cats and/or raccoon dogs. Moreover, the contribution of bromine in PBDEs to EOBr-L was >50% in two cats, while it was <6% in other specimens. This is the first report on EOBr mass balance in cetaceans and on EOX mass balance in terrestrial mammals living close to humans. These results suggest the need for analysis of unidentified chlorinated compounds in terrestrial mammals and unidentified brominated compounds in marine mammals.

Common Eider and Herring Gull as Contaminant Indicators of Different Ecological Niches of an Urban Fjord System.

Seabirds like gulls are common indicators in contaminant monitoring. The herring gull (Larus argentatus) is a generalist with a broad range of dietary sources, possibly introducing a weakness in its representativeness of aquatic contamination. To investigate the herring gull as an indicator of contamination in an urban-influenced fjord, the Norwegian Oslofjord, we compared concentrations of a range of lipophilic and protein-associated organohalogen contaminants (OHCs), Hg, and dietary markers in blood (n = 15), and eggs (n = 15) between the herring gull and the strict marine-feeding common eider (Somateria mollissima) in the breeding period of May 2017. Dietary markers showed that the herring gull was less representative of the marine food web than the common eider. We found higher concentrations of lipophilic OHCs (wet weight and lipid weight) and Hg (dry weight) in the blood of common eider (mean ± SE ∑PCB = 210 ± 126 ng/g ww, 60 600 ± 28 300 ng/g lw; mean Hg = 4.94 ± 0.438 ng/g dw) than of the herring gull (mean ± SE ∑PCB = 19.0 ± 15.6 ng/g ww, 1210 ± 1510 ng/g lw; mean Hg = 4.26 ± 0.438 ng/g dw). Eggs gave opposite results; higher wet weight and lipid weight OHC concentrations in the herring gull (mean ± SE ∑PCB = 257 ± 203 ng/g ww, 3240 ± 2610 ng/g lw) than the common eider (mean ± SE ∑PCB = 18.2 ± 20.8 ng/g ww, 101 ± 121 ng/g lw), resulting in higher OHC maternal transfer ratios in gulls than eiders. We suggest that the matrix differences are due to fasting during incubation in the common eider. We suggest that in urban areas, herring gull might not be representative as an indicator of marine contamination but rather urban contaminant exposure. The common eider is a better indicator of marine pollution in the Oslofjord. The results are influenced by the matrix choice, as breeding strategy affects lipid dynamics regarding the transfer of lipids and contaminants to eggs and remobilization of contaminants from lipids to blood during incubation, when blood is drawn from the mother. Our results illustrate the benefit of a multispecies approach for a thorough picture of contaminant status in urban marine ecosystems. Integr Environ Assess Manag 2021;17:422-433. © 2020 The Authors. Integrated Environmental Assessment and Management published by Wiley Periodicals LLC on behalf of Society of Environmental Toxicology & Chemistry (SETAC).

Lipid metabolites as indicators of body condition in highly contaminant-exposed belugas from the endangered St. Lawrence Estuary population (Canada)

The endangered St. Lawrence Estuary (SLE) beluga population is declining and has shown no sign of recovery over the past decades despite several protective measures. Changes in the availability of food resources and exposure to organohalogen contaminants have been suggested as potential factors limiting the recovery of this population. Studies on SLE belugas have suggested that contaminant exposure may perturb energy metabolism, however, whether this translates into changes in energy reserves (lipid composition) and body condition is unknown. The objective of this study was to investigate the relationships between body condition and concentrations of organohalogens (polychlorinated biphenyls, organochlorine pesticides, and flame retardants) and a range of lipid metabolites (fatty acids, acylcarnitines, lysophosphatidylcholines, phosphatidylcholines, and sphingomyelins) in blubber samples collected from 51 SLE beluga carcasses recovered between 1998 and 2016 for which the cause of mortality was documented. Blubber Σ9fatty acid concentrations in SLE belugas significantly decreased between 1998 and 2016, suggesting a decline in energy reserves over the past two decades. Concentrations of several phosphatidylcholine analogues were greater in blubber of beluga males and/or females that were in poor body condition compared to those in good body condition. Moreover, concentrations of phosphatidylcholine acyl-alkyl C32:2 were greater in females that died from primary starvation (poor body condition). Greater concentrations of Σ12emerging flame retardants were also found in blubber of SLE beluga females that were in poorer body condition. This study suggests that the use of membrane lipids including phosphatidylcholine concentrations may be a good indicator of body condition and energy reserve status in blubber of marine mammals.

A novel use of the leukocyte coping capacity assay to assess the immunomodulatory effects of organohalogenated contaminants in avian wildlife

Apex predators are characterized by high levels of biomagnifying organohalogenated contaminants (OHCs) which have been found to induce detrimental health effects in wildlife, such as immune system impairment. The leukocyte coping capacity (LCC) assay is a functional real-time measure of an innate immune response essential in pathogen resistance, known as the respiratory burst. The current study suggests the novel use of this tool to test whether OHCs impair the innate immune system of a sentinel top predator, the white-tailed eagle (Haliaeetus albicilla; WTE). The LCC analysis was performed in the field on WTE nestlings (n = 84) from northern Norway over two breeding seasons. Poly- and perfluoroalkyl substances (PFAS) dominated the total OHC load, surpassing the levels of legacy organochlorines. In addition, we detected significant negative correlations between concentrations of all polychlorinated biphenyls, p,p′-dichlorodiphenyldichloroethylene, perfluorohexane sulfonic acid and long-chain perfluorocarboxylic acids and the LCC of WTE nestlings. Based on our current findings reflecting a potential negative effect of both emerging and legacy OHCs on innate immune capacity, we suggest LCC to be a relevant and accessible test expanding the ecotoxicological toolbox to assess sub-lethal effects of OHCs in apex avian wildlife.