Publications by authors named "Adrian Covaci"

530 Publications

Humpback whales (Megaptera novaeangliae) breeding off Mozambique and Ecuador show geographic variation of persistent organic pollutants and isotopic niches.

Environ Pollut 2020 Dec 3;267:115575. Epub 2020 Sep 3.

Freshwater and Oceanic Sciences Unit of ReSearch (FOCUS - Oceanology), University of Liege, 4000, Liege, Belgium. Electronic address:

Humpback whales (Megaptera novaeangliae) from the Southern Hemisphere carry information on persistent organic pollutants (POPs) from their feeding zones in Antarctica to their breeding grounds, making this species a sentinel of contaminants accumulation in the Southern Ocean. This study aimed to evaluate driving factors, namely feeding areas, trophic level, and sex, affecting POP concentrations in the blubber of humpback whales breeding off Mozambique and off Ecuador. Biopsies of free-ranging humpback whales including blubber and skin were collected in 2014 and 2015 from Ecuador (n = 59) and in 2017 from Mozambique (n = 89). In both populations, HCB was the major contaminant followed by DDTs > CHLs > PCBs > HCHs > PBDEs. POP concentrations were significantly higher in males compared to females. HCB, DDTs, HCHs and PBDEs were significantly different between whales from the Mozambique population and the Ecuador population. Sex and feeding habits were important driving factors accounting for POP concentrations in Ecuador whales. The whales from our study had some of the lowest POP concentrations measured for humpback whales in the world. These whales fed predominantly on krill as reflected from the low δC and δN values measured in the skin. However, the isotopic niches of whales from Mozambique and Ecuador did not overlap indicating that the two populations are feeding in different areas of the Southern Ocean.
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http://dx.doi.org/10.1016/j.envpol.2020.115575DOI Listing
December 2020

Biomarkers, matrices and analytical methods targeting human exposure to chemicals selected for a European human biomonitoring initiative.

Environ Int 2021 01 20;146:106082. Epub 2020 Nov 20.

Norwegian Institute of Public Health, Norway. Electronic address:

The major purpose of human biomonitoring is the mapping and assessment of human exposure to chemicals. The European initiative HBM4EU has prioritized seven substance groups and two metals relevant for human exposure: Phthalates and substitutes (1,2-cyclohexane dicarboxylic acid diisononyl ester, DINCH), bisphenols, per- and polyfluoroalkyl substances (PFASs), halogenated and organophosphorous flame retardants (HFRs and OPFRs), polycyclic aromatic hydrocarbons (PAHs), arylamines, cadmium and chromium. As a first step towards comparable European-wide data, the most suitable biomarkers, human matrices and analytical methods for each substance group or metal were selected from the scientific literature, based on a set of selection criteria. The biomarkers included parent compounds of PFASs and HFRs in serum, of bisphenols and arylamines in urine, metabolites of phthalates, DINCH, OPFRs and PAHs in urine as well as metals in blood and urine, with a preference to measure Cr in erythrocytes representing Cr (VI) exposure. High performance liquid chromatography-tandem mass spectrometry (LC-MS/MS) was the method of choice for bisphenols, PFASs, the HFR hexabromocyclododecane (HBCDD), phenolic HFRs as well as the metabolites of phthalates, DINCH, OPFRs and PAHs in urine. Gas chromatographic (GC) methods were selected for the remaining compounds, e.g. GC-low resolution MS with electron capture negative ionization (ECNI) for HFRs. Both GC-MS and LC-MS/MS were suitable for arylamines. New developments towards increased applications of GC-MS/MS may offer alternatives to GC-MS or LC-MS/MS approaches, e.g. for bisphenols. The metals were best determined by inductively coupled plasma (ICP)-MS, with the particular challenge of avoiding interferences in the Cd determination in urine. The evaluation process revealed research needs towards higher sensitivity and non-invasive sampling as well as a need for more stringent quality assurance/quality control applications and assessments.
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http://dx.doi.org/10.1016/j.envint.2020.106082DOI Listing
January 2021

Short-term temporal variability of urinary biomarkers of organophosphate flame retardants and plasticizers.

Environ Int 2021 01 1;146:106147. Epub 2020 Nov 1.

Toxicological Center, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk, Belgium. Electronic address:

Background: Exposure to organophosphate flame retardants and plasticizers (PFRs) is commonly estimated by measuring biomarker concentrations in spot urine samples. However, their concentrations in urine can vary greatly over time due to short biological half-lives and variable exposure, potentially leading to exposure misclassification. In this study, we examined the within- and between-individual and within- and between-day variability of PFR metabolites in spot and 24-hour pooled urine samples during five consecutive days.

Methods: We collected all spot urine samples from 10 healthy adults for 5 days. On one additional day, we collected 24-hour pooled urine samples. Samples were analyzed by solid-phase extraction coupled to high-performance liquid chromatography tandem mass spectrometry. We calculated intraclass correlation coefficients (ICCs) to assess the reproducibility of metabolite concentrations in morning void and spot samples.

Results: Fair-to-good reproducibility was observed for serial measurements of bis(1,3-dichloro-2-propyl) phosphate (BDCIPP), 1-hydroxy-2-propyl bis(1-chloro-2-propyl) phosphate (BCIPHIPP), 2-hydroxyethyl bis(2-butoxyethyl) phosphate (BBOEHEP) and 2-ethyl-5-hydroxyhexyl diphenyl phosphate (5-HO-EHDPHP) (ICC: 0.396 - 0.599), whereas concentrations of diphenyl phosphate (DPHP) and 2-ethylhexyl phenyl phosphate (EHPHP) were more variable in time (ICC: 0.303 and 0.234). Reproducibility improved significantly when only morning void samples were considered and when concentrations were adjusted for urinary dilution. Collecting 24-hour pooled urine could be a reliable alternative for PFR biomarkers with poor short-term temporal variability.

Conclusions: The between-day variability was minor compared to variability observed within the same day, which suggests that collecting multiple samples could reduce exposure missclassification. Differences in the observed between- and within-individual variance were compound specific and related to both the nature of the exposure (e.g., diet vs other exposure routes, multiple sources) and the individual toxicokinetic properties of the investigated PFRs.
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http://dx.doi.org/10.1016/j.envint.2020.106147DOI Listing
January 2021

Preliminary study on the distribution of metals and persistent organic pollutants (POPs), including perfluoroalkylated acids (PFAS), in the aquatic environment near Morogoro, Tanzania, and the potential health risks for humans.

Environ Res 2021 01 13;192:110299. Epub 2020 Oct 13.

Systemic Physiological and Ecotoxicology Research (SPHERE), Department of Biology, University of Antwerp, Groenenborgerlaan 171, 2020, Antwerp, Belgium. Electronic address:

Metals and persistent organic pollutants (POPs), including perfluoroalkylated acids (PFAS), are chemicals with a bioaccumulative potential that are detected in wildlife around the world. Although multiple studies reported the pollution of the aquatic environment with these chemicals, only limited data is present on the environmental pollution of Tanzania's aquatic environment and the possible risks for human health through consumption of contaminated fish or invertebrates. In the present study, we examined the distribution of metals and POPs in fish, invertebrates, sediment and water, collected at two different years at multiple important water reservoirs for domestic and industrial purposes, in the aquatic environment near Morogoro, Tanzania. Furthermore, we assessed the possible risks for human health through consumption of contaminated fish and shrimp. Metal concentrations in the water, sediment, invertebrates and fish appeared to increase in sites downstream from Morogoro city, likely caused by the presence of the city as pollution source. Significant differences in accumulated concentrations of metals and POPs were observed between species, which was hypothesized to be caused by dietary differences. Concentrations of multiple metals exceeded water and sediment quality guidelines values. Only Cu (2.8-17 μg/L) and Zn (
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http://dx.doi.org/10.1016/j.envres.2020.110299DOI Listing
January 2021

Kinetics and biotransformation products of bisphenol F and S during aerobic degradation with activated sludge.

J Hazard Mater 2021 02 24;404(Pt A):124079. Epub 2020 Sep 24.

Jožef Stefan Institute, Jamova cesta 39, 1000 Ljubljana, Slovenia; International Postgraduate School Jožef Stefan, Jamova cesta 39, 1000 Ljubljana, Slovenia. Electronic address:

Bisphenol F (BPF) and bisphenol S (BPS) are becoming widespread in the environment despite the lack of information regarding their fate during wastewater treatment and in the environment. This study assessed the biodegradation kinetics of BPF and BPS during biological wastewater treatment with activated sludge using GC-MS/MS, and the identification of biotransformation products (BTPs) using LC-QTOF-MS. The results showed that BPF and BPS degrade readily and unlikely accumulate in biosolids or wastewater effluent (c = 0.1 mg L, half-lives <4.3 days). The first-order kinetic model revealed that BPF (k = 0.20-0.38) degraded faster than BPS (k = 0.04-0.16) and that degradation rate decreases with an increasing initial concentration of BPS (half-lives 17.3 days). The absence of any additional organic carbon source significantly slowed down degradation, in particular, that of BPS (lag phase on day 18 instead of day 7). The machine-learning algorithm adopted as part of the non-targeted workflow identified three known BTPs and one novel BTP of BPF, and one known and ten new BTPs of BPS. The data from this study support possible new biodegradation pathways, namely sulphation, methylation, cleavage and the coupling of smaller bisphenol moieties.
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http://dx.doi.org/10.1016/j.jhazmat.2020.124079DOI Listing
February 2021

Short-term variability of bisphenols in spot, morning void and 24-hour urine samples.

Environ Pollut 2021 Jan 28;268(Pt A):115747. Epub 2020 Sep 28.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610, Antwerp, Belgium. Electronic address:

Due to worldwide regulations on the application of the high production volume industrial chemical bisphenol A (BPA) in various consumer products, alternative bisphenols such as bisphenol F (BPF) and bisphenol S (BPS) are increasingly used. To assess human exposure to these chemicals, biomonitoring of urinary concentrations is frequently used. However, the short-term variability of alternative bisphenols has not been evaluated thoroughly yet, which is essential to achieve a correct estimation of exposure. In this study, we collected all spot urine samples from ten healthy adults for five consecutive days, and an additional 24 h pooled sample. We measured the concentrations of seven bisphenols (BPAF, BPF, BPA, BPB, BPZ, BPS and BPAP) in these samples using gas chromatography coupled to tandem mass spectrometry. BPA, BPF and BPS were frequently found in spot samples (>80%), while bisphenol AP (BPAP) was detected in 43% of spot samples. Calculations of intra-class correlation coefficients (ICCs) showed that reproducibility of these four bisphenols was relatively poor (<0.01-0.200) but improved when concentrations were corrected for urine dilution using creatinine levels (0.128-0.401). Of these four bisphenols, BPF showed the best reproducibility (ICC 0.200-0.439) and BPS the most variability (ICC <0.01-0.128). In general, the within-participant variability of bisphenol levels was the largest contributor to the total variance (47-100%). We compared repeated first morning voids to 24 h pooled urine and found no significantly different concentrations for BPA, BPF, BPS, or BPAP. Levels of BPA and BPF differed significantly depending on the sampling time throughout the day. The findings in this study suggest that collecting multiple samples per participant over a few days, in predefined time windows throughout the day, could result in a more reliable estimation of internal exposure to bisphenols.
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http://dx.doi.org/10.1016/j.envpol.2020.115747DOI Listing
January 2021

Early-life exposure to multiple persistent organic pollutants and metals and birth weight: Pooled analysis in four Flemish birth cohorts.

Environ Int 2020 12 28;145:106149. Epub 2020 Sep 28.

Division of Environmental Epidemiology, Institute for Risk Assessment Sciences, Utrecht University, Utrecht, the Netherlands; Julius Center for Health Sciences and Primary Care, University Medical Center Utrecht, Utrecht, the Netherlands.

Background And Aims: Prenatal chemical exposure has frequently been associated with reduced fetal growth although results have been inconsistent. Most studies associate single pollutant exposure to this health outcome, even though this does not reflect real life situations as humans are exposed to many pollutants during their life time. The objective of this study is to investigate the association between prenatal exposure to a mixture of persistent environmental chemicals and birth weight using multipollutant models.

Methods: We combined exposure biomarker data measured in cord blood samples of 1579 women from four Flemish birth cohorts collected over a 10 years' time period. The common set of available and detectable exposure measures in these cohorts are three polychlorinated biphenyls (PCB) congeners (138, 153 and 180), hexachlorobenzene (HCB), dichlorodiphenyldichloroethylene (p,p'-DDE) and the metals cadmium and lead. Multiple linear regression (MLR), Bayesian Information Criterion (BIC), penalized regression using minimax concave penalty (MCP) and Bayesian Adaptive Sampling (BAS) were applied to assess the influence of multiple pollutants in a single analysis on birth weight, adjusted for a priori selected covariates.

Results: In the pooled dataset, a median (P25-P75) birth weight and gestational age of 3420 (3140-3700) grams and 39 (39-40) weeks was observed respectively. The median contaminant levels in cord blood were: 15.8, 26.5, 18.0, 16.9 and 91.5 ng/g lipid for PCB 138, PCB 153, PCB 180, HCB and p,p'-DDE, respectively, 0.075 µg/L for cadmium and 9.7 µg/L for lead. According to the applied statistical methods for multipollutant assessment, p,p'-DDE and PCB 180 were most consistently associated with birth weight. In addition, PCB 153 was selected when applying MCP and BAS. An inverse association with birth weight was found for the PCB congeners, while an increased birth weight was observed for elevated levels of p,p'-DDE.

Conclusions: Assessing the health risk of combinations of exposure biomarkers reflects better real-world situations and thereby allows more effective risk assessment. Our results add to the existing evidence based on detrimental effects of PCBs on birth weight and indicate a possible increase in birth weight due to p,p'-DDE (while correcting for PCBs).
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http://dx.doi.org/10.1016/j.envint.2020.106149DOI Listing
December 2020

A simplified screening method for short- and medium-chain chlorinated paraffins in food by gas chromatography-low resolution mass spectrometry.

J Chromatogr A 2020 Sep 21;1631:461574. Epub 2020 Sep 21.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610, Wilrijk, Belgium. Electronic address:

This study evaluates the performance of a simplified screening method for short- and medium-chain chlorinated paraffins (SCCPs and MCCPs, respectively) based on gas chromatography-electron capture negative ionization/mass spectrometry (GC-ECNI/MS) analysis and chlorine content quantification. The response from different combinations of 'indicator' congener groups present in technical mixture standards were used within calibration calculations to test the hypothesis that ∑SCCPs and ∑MCCPs could be quantified with acceptable accuracy using only a subset of the commonly analysed C to C and Cl to Cl groups. Potential combinations were assessed with respect to calibration curve performance and accuracy of SCCP and MCCP analysis of spiked food samples (olive oil, salmon, pork sausage, breakfast cereal, cow's milk and lard). Based on these trials, a screening method which quantifies ∑SCCPs and ∑MCCPs using only congener groups with 6 and 8 chlorine atoms for each carbon chain length was proposed. Concentrations of SCCPs and MCCPs in triplicate analyses of spiked food samples calculated using the proposed screening method deviated by ≤ 25% for the vast majority of samples (maximum deviation 37%) from levels determined using all analysed congener groups. The mean trueness of the screening method as applied to each of the spiked food samples and lard samples from a previous European Union Reference Laboratory (EURL) interlaboratory study ranged from 65 to 110% for ∑SCCPs and 102 to 175% for ∑MCCPs. Relative standard deviations (RSDs) were ≤ 25% for all triplicate analyses and matrix specific LOQs ranged from 0.7 to 6 ng/g ww for ∑SCCPs and from 1.3 to 12 ng/g ww for ∑MCCPs. The proposed screening method has the potential to deliver substantial time savings in instrumental analysis and manual labour without greatly reducing the overall accuracy and sensitivity of SCCP and MCCP quantification.
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http://dx.doi.org/10.1016/j.chroma.2020.461574DOI Listing
September 2020

Between- and within-individual variability of urinary phthalate and alternative plasticizer metabolites in spot, morning void and 24-h pooled urine samples.

Environ Res 2020 12 24;191:110248. Epub 2020 Sep 24.

Toxicological Center, University of Antwerp, Universiteitsplein 1, 2610, Wilrijk, Belgium. Electronic address:

Due to international regulations, commonly used phthalates such as di(2-ethylhexyl) phthalate (DEHP) are being replaced by other phthalates, such as di-isononyl phthalate (DINP), and di-isodecyl phthalate (DIDP) and by alternative plasticizers (APs) with similar chemical characteristics, like di(isononyl)cyclohexane-1,2-dicarboxylate (DINCH), di(2-ethylhexyl) terephthalate (DEHTP), or di-(2-ethylhexyl) adipate (DEHA). Urinary concentrations of metabolites are frequently used in the exposure assessment of non-persistent chemicals and for biomonitoring purposes, the intra- and inter-day variability of the metabolites should be known. However, the short-term variability of AP and several phthalate biomarkers has not been investigated yet. In this study, we collected all spot samples from 10 healthy adults for 5 consecutive days and 24h pooled urine on one additional day to investigate the short-term variability of 22 biomarkers of phthalates and APs. Metabolites of DEP, DEHP, DiBP, DnBP, DBzP, DINP and DIDP were found in high detection frequencies, while metabolites of most APs were found in approximately 50% of the samples. The short-term reproducibility of metabolites with diet as primary source (DEHP, DINP, DIDP) was poor (intraclass correlation coefficient - ICC < 0.4), whereas biomarkers of DEP, DnBP, DiBP and BBzP showed good consistency, most likely due to more continuous sources resulting in less between-day variance. ICC values of AP metabolites were similar to those of DEHP, but more studies are required to confirm these findings. Overall, reproducibility improved considerably when values were corrected for urinary dilution and when only morning voids samples were considered. Levels in morning voids samples were consistent for 5 days and comparable to 24-h pooled urine for all metabolites except for OH-MEHTP, sum DINP and sum DIDP, which supports the use of morning voids in human biomonitoring studies.
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http://dx.doi.org/10.1016/j.envres.2020.110248DOI Listing
December 2020

Assessment of the quality of European silver eels and tentative approach to trace the origin of contaminants - A European overview.

Sci Total Environ 2020 Nov 6;743:140675. Epub 2020 Jul 6.

Laboratoire Biologie des Organismes et Ecosystèmes Aquatiques (BOREA), Muséum National d'Histoire Naturelle, CNRS FRE 2030, Sorbonne Université, IRD 207, Université de Caen Normandie, Université des Antilles, Centre de Recherche et d'Enseignement sur les Systèmes Côtiers, station de biologie marine de Dinard, 38 rue du Port Blanc, 35800 Dinard, France.

The European eel is critically endangered. Although the quality of silver eels is essential for their reproduction, little is known about the effects of multiple contaminants on the spawning migration and the European eel management plan does not take this into account. To address this knowledge gap, we sampled 482 silver eels from 12 catchments across Europe and developed methods to assess three aspects of eel quality: muscular lipid content (N = 169 eels), infection with Anguillicola crassus (N = 482), and contamination by persistent organic pollutants (POPs, N = 169) and trace elements (TEs, N = 75). We developed a standardized eel quality risks index (EQR) using these aspects for the subsample of 75 female eels. Among 169 eels, 33% seem to have enough muscular lipids content to reach the Sargasso Sea to reproduce. Among 482 silver eels, 93% were infected by A. crassus at least once during their lifetime. All contaminants were above the limit of quantification, except the 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), Ag and V. The contamination by POPs was heterogeneous between catchments while TEs were relatively homogeneous, suggesting a multi-scale adaptation of management plans. The EQR revealed that eels from Warwickshire were most impacted by brominated flame-retardants and agricultural contaminants, those from Scheldt were most impacted by agricultural and construction activities, PCBs, coal burning, and land use, while Frémur eels were best characterized by lower lipid contents and high parasitic and BTBPE levels. There was a positive correlation between EQR and a human footprint index highlighting the capacity of silver eels for biomonitoring human activities and the potential impact on the suitability of the aquatic environment for eel population health. EQR therefore represents a step forward in the standardization and mapping of eel quality risks, which will help identify priorities and strategies for restocking freshwater ecosystems.
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http://dx.doi.org/10.1016/j.scitotenv.2020.140675DOI Listing
November 2020

Biomonitoring and temporal trends of bisphenols exposure in Japanese school children.

Environ Res 2020 12 11;191:110172. Epub 2020 Sep 11.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610, Antwerp, Belgium. Electronic address:

The widely used chemical bisphenol A (BPA), applied in various consumer products, has been under scrutiny in the past 20 years due to its widespread detection in humans and potential detrimental effects on human health. Following the implementation of restrictions and phase-out initiatives, BPA has been replaced by other structurally similar bisphenols, which have not yet received the same level of research attention. In this study, we aimed to 1) investigated the internal exposure to seven bisphenols in morning void urine samples (n = 396) from 7-year-old children from Hokkaido, Japan and 2) assess possible time trends in the concentrations of bisphenols between 2012 and 2017. Information on demographic, indoor environment and dietary characteristics of participants were acquired through a self-administered questionnaire. All bisphenols were detected in the study population, with BPA, BPF and BPS showing detection frequencies >50%. Concentrations of bisphenols measured in the Japanese children in our study were generally lower compared to studies worldwide. We found that BPA concentrations decreased significantly over the study time period (average 6.5% per year), whereas BPS rose with 2.8% per year. Levels of BPA and BPF were higher in autumn compared to winter. Higher urinary BPF levels were significantly associated with higher concentrations of the oxidative stress biomarker, 8-hydroxy-2'-deoxyguanosine (8-OHdG). BPA and BPF levels were higher in children from families with lower household income. Bisphenol concentrations were significantly influenced by some other personal (e.g. household income), food intake (e.g. vegetables and cow milk) and indoor housing characteristics (e.g. flooring). This is the first study to report longitudinal time trends of bisphenols in Japan. The presented findings imply that further research on bisphenols is warranted in the future to monitor whether these time trends continue.
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http://dx.doi.org/10.1016/j.envres.2020.110172DOI Listing
December 2020

Perfluoroalkyl acids and sulfonamides and dietary, biological and ecological associations in peregrine falcons from the Laurentian Great Lakes Basin, Canada.

Environ Res 2020 12 1;191:110151. Epub 2020 Sep 1.

Ecotoxicology and Wildlife Health Division, Wildlife and Landscape Science Directorate, Environment and Climate Change Canada, L7S 1A1, Burlington, Ontario, Canada. Electronic address:

Perfluoroalkyl substances (PFAS) are a large, diverse group of chemicals and several perfluoroalkyl acids (PFAAs) are known environmental contaminants. Wildlife exposure to PFAAs and precursors has been shown, but less is known regarding replacements such as shorter-chain PFAS. In the present study, exposure to a suite of PFAAs and associations with dietary, biological and ecological factors were investigated in populations of a sentinel apex species - the peregrine falcon (Falco peregrinus). Nestling blood (n = 57) and sibling eggs (n = 9) were sampled in 2016 and 2018 from nests in rural and urban regions across the Laurentian Great Lakes Basin, Canada. PFSAs (perfluorinated sulfonic acids) including PFHxS, PFOS, and PFDS were detected in most egg and plasma samples, whereas 11 PFCAs (perfluorinated carboxylic acids; C-C, C) compared to eight PFCAs (C-C, C) were detected in most eggs and plasma, respectively. Shorter-chain C-C PFCAs were more dominant in plasma and longer-chain C-C PFCAs in eggs, but profiles were similar for PFOS, PFDS, PFUdA and PFHxDA. The exposure to PFAAs in peregrine falcons is likely mediated by dietary factors such as foraging location (δC and δS) and trophic position (δN) given the associations observed in eggs and nestling plasma, respectively. Moreover, significant relationships were observed for circulating ΣPFCAs and region (rural/urban), and nestling body condition after adjusting for sampling year and dietary tracers, suggesting that compared to rural nestlings, urban nestlings may be more exposed to ΣPFCAs and prone to their potential physiological impacts. Our findings highlight the importance of integrating dietary, biological and ecological factors when studying PFAS exposure in birds.
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http://dx.doi.org/10.1016/j.envres.2020.110151DOI Listing
December 2020

Corrigendum to "Multi-pathway human exposure assessment of phthalate esters and DINCH" [Environ. Int. 112 (2018) 115-126].

Environ Int 2020 Oct 27;143:106071. Epub 2020 Aug 27.

Department of Environmental Science and Analytical Chemistry (ACES), Stockholm University, SE-106 91 Stockholm, Sweden. Electronic address:

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http://dx.doi.org/10.1016/j.envint.2020.106071DOI Listing
October 2020

Suspect screening analysis in house dust from Belgium using high resolution mass spectrometry; prioritization list and newly identified chemicals.

Chemosphere 2021 Jan 3;263:127817. Epub 2020 Aug 3.

Toxicological Center, University of Antwerp, Universiteitsplein 1, 2610, Wilrijk, Antwerp, Belgium. Electronic address:

In recent years, several changes have been made to the composition of various products which are used indoors. Plenty of new chemical additives have been incorporated to materials to comply with current legislation and safety rules. Consequently, the emission profiles of contaminants detected indoors may change over time, requiring continuous monitoring. In this study, dust samples were collected from 25 homes located in the Flemish region of Belgium during different seasons (winter and summer). Our aim was the development of a suspect screening workflow for the identification of new chemicals which might have been applied to indoor goods, released into the indoor environment, and accumulated in dust. An in-house suspect list was curated including selected groups of compounds, namely "phthalates", "phosphates", "terephthalates", "citrates", "trimellitates", (di-, tri-, tetra-) "carboxylic acids", "adipates", "azelates", "sebacates", (di-)"benzoates", and "succinates". 63 chemicals were prioritized based on their level of identification and detection frequency in samples. Seasonal comparison was tested, indicating that higher temperatures of summer might facilitate the release of few chemicals from the products into the indoor environment. Seven chemicals, to the best of our knowledge not previously reported, were selected out of the 63 listed and identified for structure confirmation using high-resolution mass spectrometry. Tributyl trimellitate (TBTM), bis (3,5,5-trimethylhexyl) phosphate (Bis-3,5,5-TMHPh), iso-octyl 2-phenoxy ethyl terephthalate (IOPhET), dimethyl azelate (DMA), dimethyl sebacate (DMS), dipropylene glycol dibenzoate (DiPGDB) and 3,5-di-tert-butyl-4-hydroxybenzaldehyde (BHT-CHO) were detected at frequencies ranging from 8 to 52% in winter and 4-56% in summer dust.
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http://dx.doi.org/10.1016/j.chemosphere.2020.127817DOI Listing
January 2021

Quality assessment of escaping silver eel (Anguilla anguilla L.) to support management and conservation strategies in Mediterranean coastal lagoons.

Environ Monit Assess 2020 Aug 8;192(9):570. Epub 2020 Aug 8.

Dipartimento di Biologia, Università degli Studi di Roma "Tor Vergata", Rome, Italy.

Silver eel samples, collected from the lagoons of Fogliano and Caprolace (Italy), were investigated for a broad range of contaminants (29 polychlorinated biphenyls, 9 polybrominated diphenyl ethers, 5 dichlorodiphenyltrichloroethane, 5 chlordanes, hexachlorobenzene, 3 hexachlorocyclohexane, and 5 metals). Concentrations of targeted compounds stand for a general low contamination pattern. Infestation by Anguillicola crassus and virus infections were also examined. No parasite infestation was found, while infected silver eels had a low prevalence for EVEX, and, for the first time in the Mediterranean area, for AngHV-1. Overall, a good quality status of escaping silver eels, for both lagoons, was highlighted by the use of integrative Indexes. A quality assessment of the ecological status of the two lagoons was carried out developing an expert judgment approach, in order to characterize the habitat of eel stocks. A Final Pressure Index was derived, whose values showed an overall limited global anthropogenic impact acting on both lagoons. Results stand for the suitability of an integrated approach to assess lagoon habitats and eel local stocks quality. This could be proposed as a tool to identify sites yielding high quality eel spawners in the Mediterranean region, in order to set up suitable management frameworks, providing elements to appraise and discuss the potential of coastal lagoons in the Mediterranean region towards the recovery of the eel global stock.
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http://dx.doi.org/10.1007/s10661-020-08533-6DOI Listing
August 2020

Concentrations of some legacy pollutants have increased in South Australian bottlenose dolphins from 1989 to 2014.

Environ Res 2020 10 3;189:109834. Epub 2020 Jul 3.

Australian Rivers Institute (ARI), School of Environment and Science, Griffith University, Gold Coast Campus, Queensland, 4222, Australia.

Information about pollution and its potential impact in Australian marine wildlife is scarce. To fill this knowledge gap, our study investigated concentrations of legacy pollutants as well as naturally produced methoxylated polybrominated diphenyl ethers (MeO-PBDEs) in blubber, liver, kidney and muscle of Indo-Pacific bottlenose dolphins (Tursiops aduncus) from two large inverse estuaries in South Australia from 1989 to 1995 and 2009-2014. Our results show that concentrations of most pollutant classes are relatively low compared to the literature but at the higher end of the ranges reported for marine mammals in Australia. Results for some individuals exceed toxicity thresholds indicative of immunotoxicity in marine mammals. It is important to note that concentrations of some compound classes, particularly PBDEs and polychlorinated biphenyls (PCBs), increased over a time interval of 20 years thereby placing more individuals at risk in recent years. Some of the highest concentrations of persistent organic pollutants (POPs) were measured in juveniles, which may jeopardize their development and the success of future generations. These results indicate that legacy pollutants may play a role in the long-term health of T. aduncus and should be included in biomonitoring efforts.
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http://dx.doi.org/10.1016/j.envres.2020.109834DOI Listing
October 2020

A comparative study on the in vitro biotransformation of medicagenic acid using human liver microsomes and S9 fractions.

Chem Biol Interact 2020 Sep 23;328:109192. Epub 2020 Jul 23.

Toxicological Centre, Department of Pharmaceutical Sciences, University of Antwerp, Universiteitsplein 1, 2610, Antwerp, Wilrijk, Belgium. Electronic address:

Many natural products are prodrugs which are biotransformed and activated after oral administration. The investigation of gastrointestinal and hepatic biotransformation can be facilitated by in vitro screening methods. This study compares two widely used in vitro models for hepatic biotransformation: 1) human S9 fractions and 2) human liver microsomes and cytosolic fractions in a two-step sequence, with the purpose of identifying differences in the biotransformation of medicagenic acid, the putative precursor of active metabolites, responsible for the medicinal effects of the herb Herniaria hirsuta. The combination of liquid chromatography coupled to high-resolution mass spectrometry with subsequent suspect and non-target data analysis allowed the identification of thirteen biotransformation products, four of which are reported here for the first time. Eight biotransformation products resulting from oxidative Phase I reactions were identified. Phase II conjugation reactions resulted in the formation of three glucuronidated and two sulfated biotransformation products. No major differences could be observed between incubations with human liver S9 or when utilizing human microsomal and cytosolic fractions. Apart from two metabolites, both methods rendered the same qualitative metabolic profile, with minor quantitative differences. As a result, both protocols applied in this study can be used to study in vitro human liver biotransformation reactions.
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http://dx.doi.org/10.1016/j.cbi.2020.109192DOI Listing
September 2020

Legacy and emerging organophosphorus flame retardants and plasticizers in indoor microenvironments from Guangzhou, South China.

Environ Int 2020 10 21;143:105972. Epub 2020 Jul 21.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk-Antwerp, Belgium.

Indoor dust has been extensively used for assessment of indoor contamination, especially for semi-volatile organic compounds (SVOCs). In the present study, the occurrence of four groups of SVOCs, i.e. organophosphorus flame retardants (PFRs), emerging PFRs (ePFRs), legacy phthalates (LPs), and alternative plasticizers (APs), was investigated in the indoor dust and air collected from floors, table surfaces, windows, and air conditioner (A/C) filters in bedrooms and offices in Guangzhou, South China. In bedrooms, A/C filter dust showed the highest median concentrations of PFRs (4670 ng/g) and ePFRs (586 ng/g), whilst the highest median concentrations of LPs and APs were found in floor (240,880 ng/g) and window dust (157,160 ng/g), respectively. In offices, A/C filter dust showed the highest median concentrations for PFRs (6750 ng/g) and APs (504,520 ng/g), while the highest ePFR median level was found in PC table dust (5810 ng/g) and LPs in floor dust (296,270 ng/g). Median air concentrations of PFRs, ePFRs, LPs, and APs were measured at 4.6, 0.12, 399, and 25 ng/m in bedrooms, and at 8.0, 0.05, 332, and 43 ng/m in offices, respectively. Tris(1-chloro-iso-propyl) phosphate (TCIPP) was the predominant PFRs/ePFRs in both dust and air. Di(2-ethylhexyl) phthalate (DEHP), di-iso-decyl phthalate (DIDP) and di-iso-nonyl phthalate (DINP) were the main LP/AP compounds in dust, whilst di-iso-butyl phthalate (DIBP) and di-n-butyl phthalate (DNBP) were the most abundant LPs/APs in air. A significant correlation (p < 0.05) was found between dust and air levels for chemicals with log K < 14, indicating that equilibrium was achieved for these chemicals but not for those with log K > 14. Among the investigated human exposure pathways (i.e. dust ingestion, dermal absorption, and air inhalation), dust ingestion was the predominant one for all chemicals. Human exposures of this magnitude to these chemicals through the investigated pathways was unlikely to present a health risk in the present study.
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http://dx.doi.org/10.1016/j.envint.2020.105972DOI Listing
October 2020

Exposure to organophosphate esters, phthalates, and alternative plasticizers in association with uterine fibroids.

Environ Res 2020 10 9;189:109874. Epub 2020 Jul 9.

School of Public Health, Seoul National University, Seoul, Republic of Korea. Electronic address:

Exposure to endocrine disrupting chemicals is suggested to be responsible for the development or progression of uterine fibroids. However, little is known about risks related to emerging chemicals, such as organophosphate esters (OPEs) and alternative plasticizers (APs). A case-control study was conducted to investigate whether exposures to OPEs, APs, and phthalates, were associated with uterine fibroids in women of reproductive age. For this purpose, the cases (n = 32) and the matching controls (n = 79) were chosen based on the results of gynecologic ultrasonography among premenopausal adult women in Korea and measured for metabolites of several OPEs, APs, and major phthalates. Logistic regression models were employed to assess the associations between chemical exposure and disease status. Factor analysis was conducted for multiple chemical exposure assessments as a secondary analysis. Among OPE metabolites, diphenyl phosphate (DPHP), 2-ethylhexyl phenyl phosphate (EHPHP), and 1-hydroxy-2-propyl bis(1-chloro-2-propyl) phosphate (BCIPHIPP) were detected in >80% of the subjects. Among APs, metabolites of di-isononyl phthalate (DINP) and di(2-propylheptyl) phthalate (DPrHpP) were detected in >75% of the urine samples. The odds ratios (ORs) of uterine fibroids were significantly higher among the women with higher exposures to tris(1,3-dichloro-2-propyl) phosphate (TDCIPP) and tris(2-butoxyethyl) phosphate (TBOEP), di(2-ethylhexyl) terephthalate (DEHTP), DPrHpP, and di-(iso-nonyl)-cyclohexane-1,2-dicarboxylate (DINCH). In addition, urinary concentrations of mono(2-ethyl-5-oxohexyl) phthalate (MEOHP), a sum of five di(2-ethylhexyl) phthalate metabolites (∑5DEHP), and mono(4-methyl-7-hydroxyoctyl) phthalate (OH-MINP) were significantly higher in the cases. In factor analysis, a factor heavily loaded with DPrHpP and DEHP was significantly associated with uterine fibroids, supporting the observation from the single chemical regression model. We found for the first time that several metabolites of OPEs and APs are associated with increased risks of uterine fibroids among pre-menopausal women. Further epidemiological and mechanistic studies are warranted to validate the associations observed in the present study.
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http://dx.doi.org/10.1016/j.envres.2020.109874DOI Listing
October 2020

The migration of bisphenols from beverage cans and reusable sports bottles.

Food Chem 2020 Nov 18;331:127326. Epub 2020 Jun 18.

Jožef Stefan Institute, Jamova cesta 39, 1000 Ljubljana, Slovenia; International Postgraduate School Jožef Stefan, Jamova cesta 39, 1000 Ljubljana, Slovenia. Electronic address:

A precise and accurate GC-MS/MS method with ng L LLOQs, acceptable recovery (78-107%) and estimated uncertainty (U > 20%, except at LLOQ) was developed following the Eurachem guidelines. We established the migration and stability of twelve bisphenols in two food simulants (C: 20% ethanol, and B: 3% acetic acid) from beverage cans (n = 16) and reusable metal and plastic sports bottles (n = 51). Bisphenols were stable in dried (eight weeks, -20 °C) and derivatised extracts (seven days, 21 °C). Cans leached BPA (<5865 ng L), three BPF isomers (8.2-1286 ng L) and BPAP (1.6 ng L), while bottles leached BPA (<222 ng L) and BPF, BPE, BPB and BPZ (1.1-4.6 ng L). Simulant C was more aggressive than simulant B, and concentrations of bisphenols decreased with consecutive exposure to simulants. Levels of BPA migrating from cans did not exceed the specific migration limits.
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http://dx.doi.org/10.1016/j.foodchem.2020.127326DOI Listing
November 2020

Enantioselective disposition and metabolic products of isofenphos-methyl in rats and the hepatotoxic effects.

Environ Int 2020 10 11;143:105940. Epub 2020 Jul 11.

Department of Pesticide Science, College of Plant Protection, Nanjing Agricultural University, State and Local Joint Engineering Research Center of Green Pesticide Invention and Application, Nanjing, Jiangsu 210095, China. Electronic address:

Isofenphos-methyl (IFP), a chiral organophosphorus pesticide, is one of the main chemicals used to control underground insects and nematodes. Recently, the use of IFP on vegetables and fruits has been prohibited due to its high toxicity. In this study, we investigated the enantioselective distribution and metabolism of IFP and its metabolites, namely, isofenphos-methyl oxon (IFPO) and isocarbophos oxon (ICPO), in male Sprague Dawley (SD) rats. Forty eight hours (48 h) after exposure, ICPO was the main detectable compound in blood (up to 75%) and urine (up to 77%), and we found that (S)-ICPO was significantly more stable than (R)-ICPO (p < 0.05). Therefore, (S)-ICPO was proposed as a suitable candidate biomarker for the biomonitoring of IFP in human urine and blood. After 48 h exposure, 21.2-41.0%, 4.1-15.1%, and 8.6-18.7% of dosed IFP was detected in the liver of racemic, R and S enantiomer-exposed rats, respectively, and R-IFP and R-IFPO showed a faster degradation (p < 0.05). Our results showed that after one week of consecutive exposure to IFP, ICPO was accumulated in the liver of rats in both racemic and enantiopure groups (no difference between the groups, p > 0.05). We found that cytochrome P450 (CYP) (i.e. CYP2C11, CYP2D2 and CYP3A2 enzymes and carboxylesterases) is responsible for the enantioselective metabolism of IFP in liver. In addition, rats exposed to (S)-IFP exhibited hepatic lipid peroxidation, liver inflammation and hepatic fibrosis. This study provides useful information and a reference for the biomonitoring and risk assessment of IFP and organophosphorus pesticide exposure.
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http://dx.doi.org/10.1016/j.envint.2020.105940DOI Listing
October 2020

Human phase I in vitro liver metabolism of two bisphenolic diglycidyl ethers BADGE and BFDGE.

Toxicol Lett 2020 Oct 29;332:7-13. Epub 2020 Jun 29.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610, Wilrijk, Belgium. Electronic address:

Root canal sealers are commonly used to endodontically treat teeth with periapical infections. Some root canal sealers based on epoxy resin contain bisphenol A diglycidyl ether (BADGE) and bisphenol F diglycidyl ether (BFDGE). The presence of these chemicals is of concern due to the close contact to the blood stream at the apex and the long setting times of up to 24 h. These chemicals, or any of their degradation products or metabolites, can then exert their toxic effects before being excreted. This study aimed to identify the phase I in vitro biotransformation products of BADGE and BFDGE using human liver microsomes. During incubation with microsomal fractions, the epoxides were rapidly hydrolysed in a NADPH independent manner resulting in the formation of BADGE.2HO and BFDGE.2HO. Further, oxidative reactions, such as hydroxylation and carboxylation, generated other BADGE metabolites, such as BADGE.2HO-OH and BADGE.HO.COOH, respectively. For BFDGE, further oxidation of BFDGE.2HO led to the newly reported carboxylic acid, BFDGE.HO.COOH. In total, three specific metabolites have been identified which can serve in future human biomonitoring studies of BADGE and BFDGE.
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http://dx.doi.org/10.1016/j.toxlet.2020.06.022DOI Listing
October 2020

Suspect and non-targeted screening of chemicals of emerging concern for human biomonitoring, environmental health studies and support to risk assessment: From promises to challenges and harmonisation issues.

Environ Int 2020 06 29;139:105545. Epub 2020 Apr 29.

Oniris, INRAE, LABERCA, Nantes, France. Electronic address:

Large-scale suspect and non-targeted screening approaches based on high-resolution mass spectrometry (HRMS) are today available for chemical profiling and holistic characterisation of biological samples. These advanced techniques allow the simultaneous detection of a large number of chemical features, including markers of human chemical exposure. Such markers are of interest for biomonitoring, environmental health studies and support to risk assessment. Furthermore, these screening approaches have the promising capability to detect chemicals of emerging concern (CECs), document the extent of human chemical exposure, generate new research hypotheses and provide early warning support to policy. Whilst of growing importance in the environment and food safety areas, respectively, CECs remain poorly addressed in the field of human biomonitoring. This shortfall is due to several scientific and methodological reasons, including a global lack of harmonisation. In this context, the main aim of this paper is to present an overview of the basic principles, promises and challenges of suspect and non-targeted screening approaches applied to human samples as this specific field introduce major specificities compared to other fields. Focused on liquid chromatography coupled to HRMS-based data acquisition methods, this overview addresses all steps of these new analytical workflows. Beyond this general picture, the main activities carried out on this topic within the particular framework of the European Human Biomonitoring initiative (project HBM4EU, 2017-2021) are described, with an emphasis on harmonisation measures.
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http://dx.doi.org/10.1016/j.envint.2020.105545DOI Listing
June 2020

Temporal trends and determinants of PFR exposure in the Hokkaido Study.

Int J Hyg Environ Health 2020 07 17;228:113523. Epub 2020 Apr 17.

Toxicological Center, University of Antwerp, Universiteitsplein 1, 2610, Wilrijk, Belgium. Electronic address:

The phase-out of polybrominated diphenyl ethers (PBDE) flame retardants has led to the rapid increase of alternatives such as phosphate flame retardants and plasticizers (PFRs) in many consumer products. Exposure to these additive chemicals is widespread and potentially harmful to humans and the environment. In the present study, we assessed the exposure to PFRs through the analysis of metabolites in urine collected from 7-year old children from Hokkaido, Japan between 2012 and 2017. This allowed us to investigate temporal and seasonal trends for PFR metabolite concentrations and to study determinants of exposure. Thirteen metabolites of seven PFRs were measured in morning spot urine samples (n = 400). Multiple regression models were used to quantify the yearly increase in metabolite concentrations per sampling year. Information on the demographics, indoor environment and dietary habits of the participants were derived from self-administered questionnaires. PFR metabolite concentrations were comparable to our previous study of school children (7-12 years old). Eight PFR metabolites were detected in >50% of the samples. During the study time period, concentrations of three metabolites increased significantly: bis(1,3-dichloro-2-propyl) phosphate (BDCIPP; 13.3% per year), 1-hydroxy-2-propyl bis(1-chloro-2-propyl) phosphate (BCIPHIPP; 12.9% per year), and 2-ethylhexyl phenyl phosphate (EHPHP; 6.7% per year). We also found seasonality as a determinant for several PFR metabolites, with 2-fold higher levels in summer for BCIPHIPP and BDCIPP. Concentrations were also significantly impacted by ventilation habits. More frequent window opening or use of mechanical ventilation was consistently associated with higher levels of PFR metabolites in children's urine. This is the first study to show that human exposure to PFRs has increased in recent years in Japan, which indicates that further research into this class of chemicals is warranted.
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http://dx.doi.org/10.1016/j.ijheh.2020.113523DOI Listing
July 2020

Monitoring the levels of brominated and organophosphate flame retardants in passenger cars: Utilisation of car air filters as active samplers.

J Environ Sci (China) 2020 May 31;91:142-150. Epub 2020 Jan 31.

QAEHS, Queensland Alliance for Environmental Health Science, The University of Queensland, Brisbane, Australia; International Laboratory for Air Quality and Health, Queensland University of Technology, Brisbane, Australia. Electronic address:

Filters in residential and office air conditioning (A/C) systems have been used as sampling devices for monitoring different pollutants. However, cabin air filters (CAFs) in the A/C system of passenger cars have not been utilised for this purpose. In this study, we collected 22 used CAFs from passenger cars in Hanoi, Vietnam to analyse for 8 polybrominated diphenyl ethers (PBDEs) and 10 organophosphate esters (OPEs). All the analytes were detected in more than 50% of samples with the exception of BDE153 and BDE154. The average concentrations of ∑OPEs and ∑BDEs in the captured dust were 2600 and 40 ng/g, respectively with Tris (1-chloro-2-propyl) phosphate (TCIPP) and BDE209 as the dominant congener in OPE and BDE groups, respectively. CAFs are a potential tool to qualitatively assess the levels of semi-volatile chemicals in suspended dust in cars as a screening step for exposure assessment of those chemicals.
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http://dx.doi.org/10.1016/j.jes.2020.01.014DOI Listing
May 2020

Temporal trends of legacy organochlorines in different white-tailed eagle (Haliaeetus albicilla) subpopulations: A retrospective investigation using archived feathers.

Environ Int 2020 05 10;138:105618. Epub 2020 Mar 10.

Department of Bioscience, Aarhus University, Frederiksborgvej 399, PO Box 358, 4000 Roskilde, Denmark. Electronic address:

Understanding the spatiotemporal patterns of legacy organochlorines (OCs) is often difficult because monitoring practices differ among studies, fragmented study periods, and unaccounted confounding by ecological variables. We therefore reconstructed long-term (1939-2015) and large-scale (West Greenland, Norway, and central Sweden) trends of major legacy OCs using white-tailed eagle (Haliaeetus albicilla) body feathers, to understand the exposure dynamics in regions with different contamination sources and concentrations, as well as the effectiveness of legislations. We included dietary proxies (δC and δN) in temporal trend models to control for potential dietary plasticity. Consistent with the hypothesised high local pollution sources, levels of polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethanes (DDTs) and hexachlorocyclohexanes (HCHs) in the Swedish subpopulation exceeded those in the other subpopulations. In contrast, chlordanes (CHLs) and hexachlorobenzene (HCB) showed higher concentrations in Greenland, suggesting the importance of long-range transport. The models showed significantly decreasing trends for all OCs in Sweden in 1968-2011 except for CHLs, which only decreased since the 1980s. Nevertheless, median concentrations of DDTs and PCBs remained elevated in the Swedish subpopulation throughout the 1970s, suggesting that the decreases only commenced after the implementation of regulations during the 1970s. We observed significant trends of increasing concentrations of PCBs, CHLs and HCB in Norway from the 1930s to the 1970s/1980s and decreasing concentrations thereafter. All OC concentrations, except those of PCBs were generally significantly decreasing in the Greenland subpopulation in 1985-2013. All three subpopulations showed generally increasing proportions of the more persistent compounds (CB 153, p.p'-DDE and β-HCH) and decreasing proportions of the less persistent ones (CB 52, p.p'-DDT, α- and γ-HCH). Declining trends of OC concentrations may imply the decreasing influence of legacy OCs in these subpopulations. Finally, our results demonstrate the usefulness of archived museum feathers in retrospective monitoring of spatiotemporal trends of legacy OCs using birds of prey as sentinels.
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http://dx.doi.org/10.1016/j.envint.2020.105618DOI Listing
May 2020

Prenatal Exposure to Organophosphate Flame Retardants and the Risk of Low Birth Weight: A Nested Case-Control Study in China.

Environ Sci Technol 2020 03 5;54(6):3375-3385. Epub 2020 Mar 5.

Key Laboratory of Environment and Health, Ministry of Education & Ministry of Environmental Protection, State Key Laboratory of Environment Health (Incubation), School of Public Health, Tongji Medical College, Huazhong University of Science and Technology, Wuhan, 430030, China.

Organophosphate flame retardants (OPFRs), used as flame retardants and plasticizers, have been suggested to impair fetal growth and development in toxicological studies, but epidemiological data are extremely limited. This study was designed to explore whether prenatal exposure to OPFRs was associated with an increased risk of low birth weight (LBW) using a nested case-control design based on the ongoing prospective birth cohort in Wuhan, China. A total of 113 cases and 226 matched controls recruited from this cohort project in 2014-2016 were included. OPFR metabolite concentrations in maternal urine samples collected in the third trimester were determined, and birth outcomes were extracted from medical records. Compared with the lowest tertile of diphenyl phosphate (DPHP) concentrations, pregnant women with the highest tertile of DPHP had a 4.62-fold (95% confidence interval (CI): 1.72, 12.40) significantly increased risk for giving birth to LBW infants, with a significant dose-response relationship (-trend < 0.01). After stratification by newborn sex, the significant positive association of DPHP levels with LBW risk was merely observed among female newborns. Our results suggest a positive association between maternal urinary DPHP concentrations and LBW risk for the first time, and the effect appears be sex-specific.
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http://dx.doi.org/10.1021/acs.est.9b06026DOI Listing
March 2020

Combined exposure to phthalate esters and phosphate flame retardants and plasticizers and their associations with wheeze and allergy symptoms among school children.

Environ Res 2020 04 3;183:109212. Epub 2020 Feb 3.

Hokkaido University, Center for Environmental and Health Sciences, Kita 12, Nishi 7, Kita-ku, Sapporo, 060-0812, Japan. Electronic address:

Background: Phthalate esters and phosphate flame retardants and plasticizers (PFRs) are both used as plasticizers and are commonly detected in indoor environments. Although both phthalates and PFRs are known to be associated with children's wheeze and allergic symptoms, there have been no previous studies examining the effects of mixtures of these exposures.

Objectives: To investigate the association between exposure to mixtures of phthalate esters and PFRs, and wheeze and allergic symptoms among school-aged children.

Methods: A total of 128 elementary school-aged children were enrolled. Metabolites of 3 phthalate esters and 7 PFRs were measured in urine samples. Parent-reported symptoms of wheeze, rhinoconjunctivitis, and eczema were evaluated using the International Study of Asthma and Allergies in Childhood (ISAAC) questionnaire. In the primary model, we created a phthalate ester and PFR mixture exposure index, and estimated odds ratios (ORs) using weighted quantile sum (WQS) regression and quantile g (qg)-computation. The two highest chemicals according to qg-computation weight %s were combined to create a combination high × high exposure estimate, with ORs calculated using the "low × low" exposure group as the reference category. Concentrations of each metabolite were corrected by multiplying this value by the sex- and body size-Standardised creatinine concentration and dividing by the observed creatinine value. All models were adjusted for sex, grade, dampness index and annual house income.

Results: The odds ratio of rhinoconjunctivitis for the association between exposure to chemical mixtures according to the WQS index positive models was; OR = 2.60 (95% confidence interval [CI]: 1.38-5.14). However, wheeze and eczema of the WQS index positive model, none of the WQS index negative models or qg-computation result yielded statistically significant results. Combined exposure to the two highest WQS weight %s of "high-high" ΣTCIPP and ΣTPHP was associated with an increased prevalence of rhino-conjunctivitis, OR = 5.78 (1.81-18.43) to the "low × low" group.

Conclusions: Significant associations of mixed exposures to phthalates and PFRs and increased prevalence of rhinoconjunctivitis was found among elementary school-aged children in the WQS positive model. Mixed exposures were not associated with any of allergic symptoms in the WQS negative model or qg-computation approach. However, the combined effects of exposure to two PFRs suggested an additive and/or multiplicative interaction, potentially increasing the prevalence of rhinoconjunctivitis. A further study with a larger sample size is needed to confirm these results.
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http://dx.doi.org/10.1016/j.envres.2020.109212DOI Listing
April 2020

Assessment of persistent organic pollutants in hair samples collected from several Iranian wild cat species.

Environ Res 2020 04 1;183:109198. Epub 2020 Feb 1.

Toxicological Centre, University of Antwerp, 2610, Wilrijk-Antwerpen, Belgium.

Persistent organic pollutants (POPs), including the organochlorine pesticides (OCPs), such as dichlorodiphenyltrichloroethane (DDT) and its metabolites, hexachlorobenzene (HCB), α, β and γ-hexachlorocyclohexane (HCH) isomers, and the polychlorinated biphenyl (PCB) congeners (IUPAC Nos. 28, 52, 101, 138, 153, and 180), were determined in hair samples collected from 41 Iranian wild cats belonging to 8 different species. This is the first report on the presence of selected POPs in feline hair from museum collections and it is an indication of the concentrations of OCPs and PCBs in Iran from 2000 to 2010. Median concentrations of HCHs, DDTs, PCBs, and HCB were 108, 99, 70 and 38 ng/g hair, respectively. p,p'-DDE and β-HCH were the most abundant OCPs (detected in 91% and 74%, respectively, of the analyzed samples), while CB 180 and CB 138 were the predominant PCB congeners, found respectively in 49% and 61% of the samples. Significant differences (p < 0.05) in the median concentrations of DDTs were found among species grouped according to both their feeding habits and territory range. Levels of DDTs and PCBs were generally higher in the omnivorous species compared with the carnivorous ones, likely due to both their dietary habits and habitat in the proximity of human settlements.
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http://dx.doi.org/10.1016/j.envres.2020.109198DOI Listing
April 2020

Interspecies comparison of the residue levels and profiles of persistent organic pollutants in terrestrial top predators.

Environ Res 2020 04 25;183:109187. Epub 2020 Jan 25.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, Wilrijk, Belgium. Electronic address:

Serum samples from three species of living terrestrial top predators were analysed for six groups of persistent organic pollutants (POPs), such as polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethane and its metabolites (DDTs), chlordane compounds (CHLs), hexachlorocyclohexane isomers (HCHs), hexachlorobenzene (HCB) and polybrominated diphenyl ethers (PBDEs). The study included three carnivore species: lion (Panthera leo), hyena (Hyena brunnea) and cheetah (Acinonyx jubatus). All samples were collected from healthy living animals between 2004 and 2005. Most of the samples (wild lions (n = 50) and hyenas (n = 11)) were collected from various locations within the Kruger National Park and Addo National Park (South Africa), while captive lions (n = 6) and cheetahs (n = 3) were collected from the Antwerp Zoo (Belgium). In general, relatively low levels of POPs were found in the studied species, varying widely within species and locations. Median concentrations of POPs were higher in captive lions (PCBs: 505 pg/mL; DDTs: 270 pg/mL; HCHs: 72 pg/mL; HCB: 34 pg/mL; CHLs: 24 pg/mL; PBDEs: 8 pg/mL) compared to wild lions (DDTs: 274 pg/mL; HCHs: 44 pg/mL; CHLs: 7.9 pg/mL; PCBs: 2.1 pg/mL; HCB: < LOQ; PBDEs: < LOQ). In the wild animals, POPs accumulated in the following order: DDTs > HCHs > CHLs > HCB > PCBs > PBDEs, while in the captive animals, the order was: PCBs > DDTs > CHLs > HCHs > HCB > PBDEs, suggesting differences in the diet of these animals. Furthermore, wild hyena contained significantly higher (p < 0.05) median levels of POPs compared to wild lions, possibly reflecting differences in metabolic capacity and/or feeding habits, together with an uneven distribution of POPs in the area where the animals lived. No previous data are available to compare for similar terrestrial top predators, such as lion, hyena and cheetah. To our knowledge, this is first study on POPs in these three species. The low POP levels found in this study were several orders of magnitude lower than those for other carnivore species, such as polar bears, grizzly bears, brown bears and wolves worldwide. The present study has revealed the need for expanding research and monitoring on occurrence, levels and disposition of POPs in the top predators of the terrestrial environment.
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http://dx.doi.org/10.1016/j.envres.2020.109187DOI Listing
April 2020