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.

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.

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.

Immunologic, reproductive, and carcinogenic risk assessment from POP exposure in East Greenland polar bears (Ursus maritimus) during 1983-2013.

Polar bears (Ursus maritimus) are among the world's highest trophic level marine predators and as such have some of the highest tissue concentrations of organohalogen contaminants (OHCs) among Arctic biota. In this paper we present the results of a three decade (1983-2013) risk assessment of OHC exposure and effects on reproduction, immunity, and cancer (genotoxicity) in polar bears from Central East Greenland. Risk of adverse effects are evaluated using a risk quotient (RQ) approach with derivation from measured OHC concentrations in polar bear tissue and critical body residues (CBR) extrapolated for polar bears using physiologically-based pharmacokinetic modelling (PBPK). The additive RQs for all OHCs in polar bears were above the threshold for all effect categories (RQ > 1) in every year, suggesting this population has been at significant and continuous risk of contaminant-mediated effects for over three decades. RQs peaked in 1983 (RQ > 58) and again in 2013 (RQ > 50) after a period of decline. These trends follow ΣPCB levels during that time, and contributed almost all of the risk to immune, reproductive, and carcinogenic effects (71-99% of total RQ). The recent spike in RQs suggests a major shift in polar bear contaminant exposure from climate related changes in food composition and hereby the increased risk of adverse health effects. In the context of lifetime exposure ΣPCB and PFOS levels showed the interactive importance of year of birth, age, and emission history. In conclusion, the results indicate that East Greenland polar bears have been exposed to OHC levels over the period of 1983-2013 that potentially and continuously affected individual and theoretically also population health, with a peaking risk in the more recent years.

Levels and profiles of organohalogenated contaminants in human blood from Egypt.

Concentrations of polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs) and some organochlorine pesticides (OCPs) were determined in serum of Egyptian colorectal cancer patients (n = 35) and compared to a healthy control group (n = 32). p,p'-DDE (the major metabolite of DDT) was the most frequently detected contaminant with the highest concentration (median = 131 ng/g lw) in all studied serum samples. BDE-209 was the least frequently detected contaminant with a median concentration <0.3 ng/g lw. The contamination profile in patients and controls was almost identical with p,p'-DDE showing the highest median contribution (77%) and oxychlordane the lowest (1%). The low p,p'-DDT/p,p'-DDE ratio (3.7%) in serum implies bioaccumulation and past exposure to DDT (c.f. recent and ongoing intake). Statistical analysis revealed no significant differences (P > 0.05) between the levels of target contaminants in serum of patients and the control group. Gender, age and body mass index (BMI) were investigated as potential factors influencing serum contaminant levels. ΣDDT, hexachlorobenzene and pentachlorophenol concentrations showed significant positive associations with age and/or BMI of the participants. Comparison with other countries revealed concentrations of PBDEs and PCBs in Egyptian serum among the lowest reported worldwide.

Assessment of dietary exposure to organohalogen contaminants, legacy and emerging flame retardants in a Norwegian cohort.

Polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), polybrominated diphenyl ethers (PBDEs), emerging halogenated flame retardants (EHFRs) and organophosphate flame retardants (PFRs) were detected in 24h duplicate diet samples from a Norwegian cohort (n=61), with concentrations ranging from

Physiologically-based pharmacokinetic modelling of immune, reproductive and carcinogenic effects from contaminant exposure in polar bears (Ursus maritimus) across the Arctic.

Polar bears (Ursus maritimus) consume large quantities of seal blubber and other high trophic marine mammals and consequently have some of the highest tissue concentrations of organohalogen contaminants (OHCs) among Arctic biota. In the present paper we carried out a risk quotient (RQ) evaluation on OHC-exposed polar bears harvested from 1999 to 2008 and from 11 circumpolar subpopulations spanning from Alaska to Svalbard in order to evaluate the risk of OHC-mediated reproductive effects (embryotoxicity, teratogenicity), immunotoxicity and carcinogenicity (genotoxicity). This RQ evaluation was based on the Critical Body Residue (CBR) concept and a Physiologically-Based Pharmacokinetic Modelling (PBPK) approach using OHC concentrations measured in polar bear adipose or liver tissue. The range of OHC concentrations within polar bear populations were as follows for adipose, sum polychlorinated biphenyls ∑PCBs (1797-10,537 ng/g lw), sum methylsulphone-PCB ∑MeSO2-PCBs (110-672 ng/g lw), sum chlordanes ∑CHLs (765-3477 ng/g lw), α-hexachlorocyclohexane α-HCH (8.5-91.3 ng/g lw), ß-hexachlorocyclohexane ß-HCH (65.5-542 ng/g lw), sum chlorbenzenes ∑ClBzs (145-304 ng/g lw), dichlorodiphenyltrichloroethane ∑DDTs (31.5-206 ng/g lw), dieldrin (69-249 ng/g lw), polybrominated diphenyl ethers ∑PBDEs (4.6-78.4 ng/g lw). For liver, the perfluorooctanesulfonic acid (PFOS) concentrations ranged from 231-2792 ng/g ww. The total additive RQ from all OHCs ranged from 4.3 in Alaska to 28.6 in East Greenland bears for effects on reproduction, immune health and carcinogenicity, highlighting the important result that the toxic effect threshold (i.e. RQ>1) was exceeded for all polar bear populations assessed. PCBs were the main contributors for all three effect categories, contributing from 70.6% to 94.3% of the total risk and a RQ between 3.8-22.5. ∑MeSO2-PCBs were the second highest effect contributor for reproductive and immunological effects (0.17

Thyroid hormones and deiodinase activity in plasma and tissues in relation to high levels of organohalogen contaminants in East Greenland polar bears (Ursus maritimus).

Previous studies have shown relationships between organohalogen contaminants (OHCs) and circulating levels of thyroid hormones (THs) in arctic wildlife. However, there is a lack of knowledge concerning the possible functional effects of OHCs on TH status in target tissues for TH-dependent activity. The relationships between circulating (plasma) levels of OHCs and various TH variables in plasma as well as in liver, muscle and kidney tissues from East Greenland sub-adult polar bears (Ursus maritimus) sampled in 2011 (n=7) were therefore investigated. The TH variables included 3.3',5.5'-tetraiodothyronine or thyroxine (T4), 3.3',5-triiodothyronine (T3) and type 1 (D1) and type 2 (D2) deiodinase activities. Principal component analysis (PCA) combined with correlation analyses demonstrated negative relationships between individual polychlorinated biphenyls (PCBs) and their hydroxylated (OH-) metabolites and T4 in both plasma and muscle. There were both positive and negative relationships between individual OHCs and D1 and D2 activities in muscle, liver and kidney tissues. In general, PCBs, OH-PCBs and polybrominated dipehenyl ethers (PBDEs) were positively correlated to D1 and D2 activities, whereas organochlorine pesticides and byproducts (OCPs) were negatively associated with D1 and D2 activities. These results support the hypothesis that OHCs can affect TH status and action in the target tissues of polar bears. TH levels and deiodinase activities in target tissues can be sensitive endpoints for exposure of TH-disrupting compounds in arctic wildlife, and thus, tissue-specific responses in target organs should be further considered when assessing TH disruption in wildlife studies.

The effect of organohalogen contaminants on western Steller sea lion survival and movement in the Russian Far East.

The western stock of Steller sea lions (Eumetopias jubatus) have experienced dramatic declines since the 1960s, particularly in the western Alaskan and Asian portions, which have continued to decline or stabilized at low levels. Multiple causes for this decline have been proposed and may include anthropogenic contamination from organohalogen contaminants (OCs). These include polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethane (DDT), which have not been ruled out as a potential cause for the lack of recovery. The objective of this study was to determine the effects of OCs on survival and movement probabilities estimated in program MARK using resighting data collected from 2003 to 2009. PCBs and DDTs were measured in whole blood from 136 (74 males and 62 females) individually marked, free-ranging pups from four Russian Far East rookeries. The mean concentration of ∑PCB and ∑DDT was 4.25±5.12 and 3.22±4.28 ng g(-1) ww (n=136), respectively, and the average ∑PCB and ∑DDT concentration for those above the aggregate mean (n=44) was 9.25±6.55 and 7.65±5.21 ng g(-1) ww, and those below the aggregate mean (n=92) the concentration was 1.86±0.89 and 1.11±0.65 ng g(-1) ww, respectively. The lowest estimated probabilities of survival occurred in the first year, ranging from 38% to 74%, but increased for ages 1-9, ranging from 82% to 94%. The greatest movement occurred from Medny Island west toward the Kamchatka Peninsula (33%) and to Bering Island (18%), and low movement estimates for other natal rookeries was largely due to minimal resighting effort. The estimated probabilities of resighting varied by location (48%-87%), but had greater precision than survival or movement parameters. Survival and movement were most affected by age and location rather than OCs.

Altered vitamin D status in liver tissue and blood plasma from Greenland sledge dogs (Canis familiaris) dietary exposed to organohalogen contaminated minke whale (Balaenoptera acuterostrata) blubber.

This study compared vitamin D3 (vitD3) and 25-OH vitamin D3 (25OHD3) status in Greenland sledge dogs (Canis familiaris) given either minke whale (Balaenoptera acuterostrata) blubber high in organohalogen contaminants (OHCs) or clean porcine (Suis scrofa) fat for up to 636 days. A group of six exposed and six control sister bitches (maternal generation) and their three exposed and four control pups, respectively, were daily fed 112g whale blubber (193µg ∑PCB/day) or porcine fat (0.17µg ∑PCB/day). Mean level of ∑PCB in adipose tissue of exposed bitches and their pups was 3106 and 2670ng/g lw, respectively, which was significantly higher than the mean concentration of 53ng/g lw for all controls (p<0.001). The vitamin analyses showed that 25OHD3 in liver of maternal exposed bitches were significantly lower than in controls (p=0.004) while vitD3 was significantly highest in liver of exposed pups (p<0.003). Regarding blood plasma concentrations, exposed F generation pups had significantly higher concentrations of 25OHD3 than controls (p=0.009). Correlation analyses showed that blood 25OHD3 decreased significantly with increased adipose tissue concentrations of ∑PCB in exposed dogs (R(2)=0.64, p=0.005) and a similar trend was found for liver 25OHD3 (R(2)=0.32, p=0.08). The results indicate that the homeostasis and metabolism of vitamin D compounds may respond differently to the dietary composition of fatty acids and OHC exposure. It is unknown if the lower level of 25OHD3 in the liver of exposed dogs would have any negative effects on immunity and reproduction and more focus should be conducted on this compound in Arctic wildlife.