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Abstract: The present study investigated the current-use brominated flame retardants (BFRs) tetrabromobisphenol A (TBBPA) and hexabromocyclododecane (HBCD), simultaneously with legacy polybrominated diphenyl ethers (PBDEs), in Barn Owls (Tyto alba) collected from two regions with a contrasting degree of urbanisation and vicinity to point sources (Flanders in Belgium versus Normandy in France). Both tissues (muscle, liver, adipose and preen gland) and feathers (primary, tail and body feathers) showed elevated HBCD concentrations in Flanders, close to Europe's sole HBCD production plant in the Netherlands, and identified Normandy as a historical source region for PBDEs. In sharp contrast, the reactive BFR TBBPA bioaccumulated poorly (2.3%) in tissue samples, but was present in 96% of all body feather samples (0.36–7.07ngg−1 dw), equally in both regions. PBDE concentrations in tissues (7.46–903ngg−1 lw) were considerably lower in the investigated Flemish Barn Owls, collected in 2008/2009, compared to specimens collected in 2003/2004 (46–11,000ngg−1 lw), possibly suggesting the effectiveness of the 2004 European ban of Penta- and Octa-BDE mixtures. Feathers showed a similar trend and additionally exhibited HBCD concentrations (0.02–333ngg−1 dw) surpassing those of PBDEs (0.50–10.4ngg−1 dw). While body feathers were a reliable matrix to predict both internal PBDE (0.21≤ R 2 ≤0.67) and HBCD body burdens (0.20≤ R 2 ≤0.37), the suitability of primary and tail feathers appeared to be confounded by external contamination and moult. In conclusion, the present study clearly showed that the reactive versus additive use of BFRs results in contrasting exposure scenarios in a species higher up the food chain, and therefore may have profound implications for environmental health. In addition, the presented results extend the promising use of feathers as a non-destructive sampling strategy for current-use BFRs, and show that birds of prey are valid early-warning systems for environmental contamination. [Copyright &y& Elsevier]

Abstract: Large-scale international monitoring studies are important to assess emission patterns and environmental distributions of organohalogenated contaminants (OHCs) on a worldwide scale. In this study, the presence of OHCs was investigated on three continents (Europe, North America and Australasia), using eggs of starlings (Sturnus vulgaris and Sturnus unicolor) to assess their suitability for large-scale monitoring studies. To the best of our knowledge, this is the first study using bird eggs of the same species as a biomonitor for OHCs on an intercontinental scale. We found significant differences in OHC concentrations of the eggs among sampling locations, except for hexachlorocyclohexanes (HCHs). Mean concentrations of sum polychlorinated biphenyls (PCBs) in eggs ranged from 78±26ng/glipid weight (lw) in Australia to 2900±1300ng/glw in the United States. The PCB profile was dominated by CB 153 and CB 138 in all locations, except for New Zealand, where the contribution of CB 95, CB 101 and CB 149 was also high. The highest mean sum polybrominated diphenyl ether (PBDE) concentrations were found in Canada (4400±830ng/glw), while the lowest mean PBDE concentrations were measured in Spain (3.7±0.1ng/glw). The PBDE profile in starling eggs was dominated by BDE 47 and BDE 99 in all countries, but in Belgium, the higher brominated PBDEs had a higher contribution compared to other countries. For the organochlorine pesticides (OCPs), dichlorodiphenyltrichloroethanes (DDTs) ranged from 110±16ng/glw in France to 17,000±3400ng/glw in New Zealand, while HCHs and hexachlorobenzene were generally in low concentrations in all sampling locations. Chlordanes were remarkably high in eggs from the United States (2500±1300ng/glw). The OCP profile in all countries was largely dominated by p,p′-DDE. In general, the worldwide trends we observed in starling eggs were in accordance with the literature on human and environmental OHC data, which suggests that there is potential for using starling eggs as a biomonitoring tool on a large geographical scale. [Copyright &y& Elsevier]

Although eggs have frequently been used as a biomonitoring tool for contamination with organohalogenated pollutants (OHPs), few studies have investigated the processes of maternal transfer in birds. Here, maternal transfer of polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs) and polybrominated diphenyl ethers (PBDEs) was investigated through comparison of the concentrations and profiles between whole homogenised female blue tits (Cyanistes caeruleus) and their eggs. In addition, we examined if there was an effect of laying order on the concentrations of PCBs, OCPs and PBDEs. PCBs were the most abundant contaminants in female blue tits and their eggs, followed by OCPs and PBDEs. Among the OCPs, p,p′-DDE was the most dominant compound and accounted for more than 80% of the sum OCPs. Egg concentrations decreased significantly in relation to the laying order from 1623±148 ng/g lipid weight (lw) to 1040±47 ng/g lw for the sum PCBs, from 342±24 ng/g lw to 235±17 ng/g lw for the sum OCPs and from 49±5 ng/g lw to 27±5 ng/g lw for the sum PBDEs. When reviewing all studies investigating laying order effects of OHPs in birds, no clear patterns emerged, which may be due to differences in study species and methodology among studies. Despite the fact that there were laying order effects in blue tit clutches, the variance in concentrations of PCBs and PBDEs was larger among clutches than within clutches. Variance in OCP concentrations among clutches was similar to the variance within clutches. These results suggest that one randomly collected blue tit egg from a clutch is useful as biomonitoring tool for PCBs and PBDEs, while for OCPs it is recommended to consistently use the same egg from the laying sequence as a biomonitoring tool. Lipid-normalized concentrations of sum PCBs, sum OCPs and sum PBDEs in female blue tits after clutch completion were comparable to the concentrations in the first-laid eggs. The egg/female lipid... [Copyright &y& Elsevier]

Abstract: We investigated the possible sources of contamination with organic pollutants, such as polychlorinated biphenyls (PCBs), p,p′-dichlorodiphenyltrichloroethane (DDT) and metabolites, and polybrominated diphenyl ethers (PBDEs), in and onto tail feathers of a large songbird, the common magpie (Pica pica). Although feathers are potentially useful as a non-destructive biomonitor for organic pollutants, concentrations may be influenced by external contamination onto the feather surface. In a first approach, a group of magpies was captured after the completion of moult. The third tail feather was pulled out and a blood sample was taken. Most PCBs, DDTs and some PBDEs could be quantified in one single tail feather, indicating that the applicability of feathers goes beyond monitoring with predatory birds, as shown previously. Nevertheless, correlations between levels in serum and feathers were found significant in three cases only (i.e. CB 170, CB 180 and CB 187). This finding may be attributed to different factors, such as varying diet, condition, sample size or external contamination. In a second approach, cadavers of magpies were collected throughout Flanders. The preen gland was removed and the first, third and fifth tail feathers were pulled out at both sides. No significant differences were found among tail feathers within an individual. We compared three washing procedures to remove external contamination with organic pollutants from these feathers: deionised water, acetone and a surfactant/acetone solution. Right feathers were washed and left feathers were kept as control. Concentrations in the resulting washes were found highest in the acetone solutions. Furthermore, feathers washed with acetone or with a surfactant/acetone solution had significantly lower mean concentrations than the control feathers. Highest correlations with levels in preen gland were obtained for the control feathers. Consequently, the source of external contamination with organic pollutants onto feathers seems to be endogenous, originating from the preen gland. This is in great contrast to the extensive airborne pollution that has been reported for most heavy metals. In summary, the results of the current study highlight the usefulness of feathers for non-destructive biomonitoring of organic pollutants. [Copyright &y& Elsevier]

Small-scale geographical variation in the occurrence of polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs) and polybrominated diphenyl ethers (PBDEs) was investigated using the eggs of a terrestrial residential songbird species, the great tit (Parus major). In addition, we investigated the influence of the type of sampling location on the presence of these pollutants. To achieve this, 10 different sampling locations in Flanders (Belgium) were classified into 3 groups based on the extent of urbanisation, industrialisation and agriculture. The higher variance among sampling locations for the levels and profiles of PCBs and OCPs, suggests that local contamination sources are more important for the PCBs and OCPs compared to the PBDEs. Levels of PCBs and PBDEs were significantly higher in the industrialised sampling locations compared to the other locations. Sum PCB and sum PBDE levels reached up to 6050 and 79 ng/g lipid weight, respectively. PCBs and PBDEs were highly positively correlated for all groups, suggesting similar exposure pathways and/or mechanisms of accumulation. Significantly higher levels of OCPs (sum OCPs up to 2683 ng/g lipid weight) were detected in the rural sampling locations situated in a residential area. This suggests that local historical usage of OCPs by inhabitants may be an important source of contamination in Flanders. Contamination profiles differed also among the sampling locations. The rural sampling locations had a higher contribution of lower brominated BDE congeners, whereas the industrialised locations had a higher contribution of higher brominated congeners. The differences in contamination profiles among the sampling locations are probably due to differences in exposure. In conclusion, our results showed that the characteristics of a sampling location influence both the levels and profiles of PCBs, OCPs and PBDEs. [Copyright &y& Elsevier]

Abstract: In this study, concentrations and profiles of organic pollutants were investigated in a passerine species with a large clutch size, the great tit (Parus major). In the first clutches, mean egg concentrations decreased significantly in relation to the laying order from 3025±416 ng/g lw to 2267±386 ng/g lw for sum PCBs and from 989±339 ng/g lw to 695±320 ng/g lw for sum DDTs. Sum PBDE concentrations also decreased in relation to the laying order from 68±10 ng/g lw to 53±11 ng/g lw, but not significantly. Although laying order effects were found, variation in concentrations within clutches was smaller than among clutches. To further investigate the impact of laying large numbers of eggs on levels and profiles of organic pollutants, initiation of replacement clutches was experimentally induced. Mean sum PCB and sum PBDE concentrations were significantly lower in eggs of replacement clutches compared to first clutches. In addition, first clutches had a higher contribution of the higher chlorinated and more persistent PCB congeners, CB 170, 180 and 183, and a lower contribution of CB 52, 95 and 149 compared to replacement clutches. Because of the differences in concentrations and profiles between the first and replacement clutches, the combined use of eggs from both the first and replacement clutches for monitoring purposes is not recommended. In conclusion, we suggest that, due to the larger variation among clutches compared to the variation within clutches, one randomly collected great tit egg from a first clutch is useful as a biomonitoring tool for organic pollutants. To our knowledge, this is the first study in which the impact of an experimentally increased clutch size on the levels and profiles of contaminants in eggs has been investigated. [Copyright &y& Elsevier]

Large-scale studies are essential to assess the emission patterns and spatial distribution of organohalogenated pollutants (OHPs) in the environment. Bird eggs have several advantages compared to other environmental media which have previously been used to map the distribution of OHPs. In this study, large-scale geographical variation in the occurrence of OHPs, such as polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs), was investigated throughout Europe using eggs of a terrestrial residential passerine species, the great tit (Parus major). Great tit eggs from 22 sampling sites, involving urban, rural and remote areas, in 14 European countries were collected and analysed (5–8 eggs per sampling site). The environmentally most important congeners/compounds of the analysed pollutants were detectable in all sampling locations. For PCBs, PBDEs and OCPs, no clear geographical contamination pattern was found. Sum PCB levels ranged from 143 ng/g lipid weight (lw) to 3660 ng/g lw. As expected, PCB concentrations were significantly higher in the sampled urban compared to the remote locations. However, the urban locations did not show significantly higher concentrations compared to the rural locations. Sum PBDEs ranged from 4.0 ng/g lw to 136 ng/g lw. PBDEs were significantly higher in the urbanized sampling locations compared to the other locations. The significant, positive correlation between PCB and PBDE concentrations suggests similar spatial exposure and/or mechanisms of accumulation. Significantly higher levels of OCPs (sum OCPs ranging from 191 ng/g lw to 7830 ng/g lw) were detected in rural sampling locations. Contamination profiles of PCBs, PBDEs and OCPs differed also among the sampling locations, which may be due to local usage and contamination sources. The higher variance among sampling locations for the PCBs and OCPs, suggests that local contamination sources are more important for the PCBs and... [Copyright &y& Elsevier]

Abstract Biomagnification of Hg and persistent organic pollutants (POPs: polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), polybrominated diphenyl ethers (PBDEs)) in aquatic food chains can lead to high pollutant concentrations in top predators, including humans. Despite this threat to human health, research concerning bioaccumulation is still underrepresented in the southern hemisphere and in (sub)arctic and (sub)tropical areas, emphasizing the need for research in these locations. In this study, samples of water, sediment and aquatic biota were analyzed to determine concentrations of POPs and total mercury (THg) in the Ga-Selati river (South Africa) and two rivers Rena and Gudbrandsdalslågen in Norway. Trophic magnification factors (TMFs) were determined to evaluate and compare the biomagnification and the threat to human health due to consumption of the fish was assessed. Concentrations of POPs in sediment and biota samples were generally low except for relatively high concentrations of ∑DDX (dichlorodiphenyltrichloroethane and metabolites) in aquatic biota from the Ga-Selati river (ranging from 1.9 to 133 ng/g ww in invertebrates and 1.9 to 5643 ng/g ww in fish). Dissolved THg concentrations were high in the Ga-Selati river (ranging from 0.009 to 0.036 μg/l) but THg concentrations in sediment and biota were low in studied rivers compared to other studies. Biomagnification occurred for THg, several DDT-metabolites and PCB compounds, TN and CN. Biomagnification of p,p′ -DDT and THg differed significantly between the two countries, supporting existing patterns found in literature, although more data is needed to attribute these differences to climatic or other factors. Concentrations in fish from the rivers Ga-Selati and Rena were under the threshold levels reported for THg and POPs, but caution should be taken when consuming Northern pike (Esox Lucius) from the subarctic river Gudbrandsdalslågen, to avoid harmful effects due to both elevated THg and PBDE exposure. Graphical abstract Unlabelled Image Highlights • POPs and Hg biomagnify ls in the river ecosystems of the Ga-Selati (South Africa), Rena and Laagen (Norway). • Overall low concentrations in water, sediment and aquatic biota • Biomagnification of Hg and pp ′-DDT differs significantly between the two climates. • Levels of Hg and PBDE in Northern pike (river Laagen) is of concern to human health. [ABSTRACT FROM AUTHOR]

Exposure to persistent organic pollutants (POPs), such as organochlorines (OCs) and polybrominated diphenyl ethers (PBDEs), is associated with adverse health effects in wildlife. Many POPs have been banned and consequently their environmental concentrations have declined. To assess both temporal trends of POPs and their detrimental impacts, raptors are extensively used as biomonitors due to their high food web position and high contaminant levels. White-tailed eagles (WTEs; Haliaeetus albicilla) in the Baltic ecosystem represent a sentinel species of environmental pollution, as they have suffered population declines due to reproductive failure caused by severe exposure to dichlorodiphenyltrichloroethane (DDT) and polychlorinated biphenyls (PCB) during the 1960s through 1980s. However, there is a lack of long-term studies that cover a wide range of environmental contaminants and their effects at the individual level. In this study, we used 135 pooled samples of shed body feathers collected in 1968–2012 from breeding WTE pairs in Sweden. Feathers constitute a temporal archive for substances incorporated into the feather during growth, including corticosterone, which is the primary avian glucocorticoid and a stress-associated hormone. Here, we analysed the WTE feather pools to investigate annual variations in feather corticosterone (fCORT), POPs (OCs and PBDEs), and stable carbon and nitrogen isotopes (SIs; dietary proxies). We examined whether the expected fluctuations in POPs affected fCORT (8–94 pg. mm−1) in the WTE pairs. Despite clear temporal declining trends in POP concentrations (p < 0.01), we found no significant associations between fCORT and POPs or SIs (p > 0.05 in all cases). Our results do not support fCORT as a relevant biomarker of contaminant-mediated effects in WTEs despite studying a highly contaminated population. However, although not detecting a relationship between fCORT, POP contamination and diet, fCORT represents a non-destructive and retrospective assessment of long-term stress physiology in wild raptors otherwise not readily available. • Use of feathers of a sentinel bird in the Baltic Sea as decadal archives of pollution. • Use of feather corticosterone fCORT as a retrospective measure of stress physiology. • Investigation of relationship between fCORT and organic pollutants in adult eagles. • Clear decreasing trends in legacy pollutants but no relationships with fCORT. • Stress factors other than exposure to pollutants may impact fCORT. [ABSTRACT FROM AUTHOR]

The occurrence of organohalogenated compounds (OHCs) in wildlife has received considerable attention over the last decades. Among the matrices used for OHCs biomonitoring, feathers are particularly useful as they can be collected in a minimally or non-invasive manner. In this study, concentrations of various legacy OHCs –polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs) and polybrominated diphenyl ethers (PBDEs)–, as well as emerging OHCs –per- and polyfluoroalkyl substances (PFAS) and organophosphate ester flame retardants (OPEs)– were determined in feathers of 72 Eurasian eagle-owls (Bubo bubo) from Norway, with the goal of studying spatiotemporal variation using a non-invasive approach. Molted feathers were collected at nest sites from northern, central and southern Norway across four summers (2013–2016). Additionally, two museum-archived feathers from 1979 to 1989 were included. Stable carbon (δ13C) and nitrogen isotopes (δ15N) were used as dietary proxies. In total, 11 PFAS (sum range 8.25–215.90 ng g−1), 15 PCBs (4.19–430.01 ng g−1), 6 OCPs (1.48–220.94 ng g−1), 5 PBDEs (0.21–5.32 ng g−1) and 3 OPEs (4.49–222.21 ng g−1) were quantified. While we observed large variation in the values of both stable isotopes, suggesting a diverse diet of the eagle-owls, only δ13C seemed to explain variation in PFAS concentrations. Geographic area and year were influential factors for δ15N and δ13C. Considerable spatial variation was observed in PFAS levels, with the southern area showing higher levels compared to northern and central Norway. For the rest of OHCs, we observed between-year variations; sum concentrations of PCBs, OCPs, PBDEs and OPEs reached a maximum in 2015 and 2016. Concentrations from 1979 to 1989 were within the ranges observed between 2013 and 2016. Overall, our data indicate high levels of legacy and emerging OHCs in a top predator in Norway, further highlighting the risk posed by OHCs to wildlife. • Assessment of legacy and emerging OHCs in feathers of Norwegian eagle-owls. • Exploration of spatiotemporal variations and association with dietary proxies. • High concentrations of both legacy and emerging OHCs are found. • Spatial variation is observed for PFAS, while POPs and OPEs show between-year variation. [ABSTRACT FROM AUTHOR]

Abstract: To circumvent difficulties associated with monitoring adult predatory birds, we investigated the feasibility of different non-destructive strategies for nestling white-tailed eagles (Haliaeetus albicilla). We were able to quantify polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorinated pesticides (OCPs) in body feathers (16.92, 3.37 and 7.81ngg−1 dw, respectively), blood plasma (8.37, 0.32 and 5.22ngmL−1 ww, respectively), and preen oil (1157.95, 30.92 and 440.74ngg−1 ww, respectively) of all nestlings (N=14). Strong significant correlations between blood plasma and preen oil concentrations (0.565≤r≤0.801; P<0.05) indicate that preen oil levels closely reflect the internal state of contamination. We found fewer significant correlations between body feather and blood plasma concentrations, which were almost exclusively between PCB concentrations (0.554≤r≤0.737; P<0.05). These results differ from a previous study on younger nestlings, and may indicate that the nestlings studied here, ready to fledge the nest, were possibly undergoing certain physiological changes that may have confounded the use of body feathers as biomonitor matrix. Finally, we provide an integrated discussion on the use of body feathers and preen oil as non-destructive biomonitor strategies for nestling predatory birds. [Copyright &y& Elsevier]

Environmental exposure to organohalogenated contaminants (OHCs), even at low concentrations, may cause detrimental effects on the development and health of wild birds. The present study investigated if environmental exposure to OHCs may influence the variation of multiple physiological parameters in Norwegian white-tailed eagle (Haliaeetus albicilla) nestlings. Plasma and feather samples were obtained from 70 nestlings at two archipelagos in Norway in 2015 and 2016. The selected physiological parameters were plasma concentrations of thyroid hormones (thyroxine, T4 and triiodothyronine, T3), plasma proteins (prealbumin, albumin, α 1 -, α 2 -, β- and γ-globulins) and selected blood clinical chemical parameters (BCCPs) associated with liver and kidney functioning. Feather concentrations of corticosterone (CORT f) were also included to investigate the overall stress level of the nestlings. Concentrations of all studied physiological parameters were within the ranges of those found in other species of free-living birds of prey nestlings and indicated that the white-tailed eagle nestlings were in good health. Our statistical models indicated that perfluoroalkyl substances (PFASs) and legacy OHCs, such as polychlorinated biphenyls, organochlorinated pesticides and polybrominated diphenyl ethers, influenced only a minor fraction of the variation of plasma thyroid hormones, prealbumin and CORT f (5–15%), and partly explained the selected BCCPs (<26%). Most of the variation in each studied physiological parameter was explained by variation between nests, which is most likely due to natural physiological variation of nestlings in these nests. This indicates the importance of accounting for between nest variation in future studies. In the present nestlings, OHC concentrations were relatively low and seem to have played a secondary role compared to natural variation concerning the variation of physiological parameters. However, our study also indicates a potential for OHC-induced effects on thyroid hormones, CORT f , prealbumin and BCCPs, which could be of concern in birds exposed to higher OHC concentrations than the present white-tailed eagle nestlings. • Several physiological parameters were investigated in white-tailed eagle nestlings. • The parameters were mostly influenced by temporal, spatial and among nest variation. • The white-tailed eagle nestlings had low OHC burdens and seemed to be in good health. • These low OHCs burdens had a minor influence on the selected physiological parameters. [ABSTRACT FROM AUTHOR]