Recycling plastics containing decabromodiphenyl ether into new consumer products including children's toys purchased in Japan and seventeen other countries.

Polybrominated diphenyl ethers (PBDEs) are flame retardants widely used to manufacture several commercial plastic products. The major homologue in commercial PBDE mixtures are listed in the Stockholm Convention on Persistent Organic Pollutants and are scheduled for global elimination. Hence, to understand more about unintentional contamination of plastic recycling stream by restricted PBDEs, we examined 540 small plastic consumer products (1139 components after dismantling), including children's toys, purchased in 18 countries (mainly Japan) between 2015 and 2019. Handheld X-ray fluorescence analysis revealed that 219 plastic components (19% of the total samples) contained bromine at a concentration of ≥30 mg kg-1. Chemical analysis of these bromine-positive components revealed that 109 pieces (9.6% of the total), mainly those made of black-colored plastic, contained PBDEs at concentrations ranging between 35 and 10,000 mg kg-1, with the maximum contribution from decabromodiphenyl ether (decaBDE). These PBDE concentrations were insufficient to impart flame retardancy, suggesting that the recycled plastic used to manufacture these consumer products probably originated from electronic waste, the manufacture of which was the primary use of commercial decaBDE mixtures. PBDEs were also found in secondary raw plastic materials and their final products obtained in India in 2019, demonstrating that plastics containing decaBDE end up in products where they serve no functional purpose. To contribute to the circular economy, the recycling of plastic waste in end-of-life products should be promoted. However, urgent action is needed to prevent plastic additives of concern, including PBDEs, from entering new products used in daily lives, particularly those used by children.

Antiandrogenic and Estrogenic Activity Evaluation of Oxygenated and Nitrated Polycyclic Aromatic Hydrocarbons Using Chemically Activated Luciferase Expression Assays.

To establish the risk of the endocrine disrupting activity of polycyclic aromatic compounds, especially oxygenated and nitrated polycyclic aromatic hydrocarbons (oxy-PAHs and nitro-PAHs, respectively), antiandrogenic and estrogenic activities were determined using chemically activated luciferase expression (CALUX) assays with human osteoblast sarcoma cells. A total of 27 compounds including 9 oxy-PAHs (polycyclic aromatic ketones and quinones) and 8 nitro-PAHs was studied. The oxy-PAHs of 7H-benz[de]anthracen-7-one (BAO), 11H-benzo[a]fluoren-11-one (B[a]FO), 11H-benzo[b]fluoren-11-one (B[b]FO), and phenanthrenequinone (PhQ) exhibited significantly the potent inhibition of AR activation. All nitro-PAHs exhibited high antiandrogenic activities (especially high for 3-nitrofluoranthene (3-NFA) and 3-nitro-7H-benz[de]anthracen-7-one (3-NBAO)), and the AR inhibition was confirmed as noncompetitive for 3-NFA, 3-NBAO, and 1,3-dinitropyrene (1,3-DNPy). Antiandrogenic activity of 3-NFA demonstrated characteristically a U-shaped dose-response curve; however, the absence of fluorescence effect on the activity was confirmed. The prominent estrogenic activity dependent on dose-response curve was confirmed for 2 oxy-PAHs (i.e., B[a]FO and B[b]FO). Elucidating the role of AR and ER on the effects of polycyclic aromatic compounds (e.g., oxy- and nitro-PAHs) to endocrine dysfunctions in mammals and aquatic organisms remains a challenge.

The effects of 28-day early-life exposure to triphenyl phosphate (TPhP) on odor preference and sexual behavior in female rats.

Many chemical substances are detectable in house dust, and they are consequently taken into our bodies via the mouth and nose. Triphenyl phosphate (TPhP), a flame retardant that has an estrogen-like effect in vitro, is present in house dust at high concentrations. Estrogen exposure during development has significant influences on reproductive behavior in rodents, and its effects persist until maturity. In the present study, we investigated the effect of early life exposure to TPhP on the reproductive behavior of female rats. Oral treatment with TPhP (25 or 250 mg/kg), ethinyl estradiol (EE; 15 µg/kg) as a positive control, or sesame oil as a negative control, were given to female rats (from birth to 28 days of age). The 8-week-old rats were bilaterally ovariectomized. At 12-15 weeks of age, the rats were subjected to odor preference and sexual behavior tests. In the odor preference test, the oil group showed significantly higher preference for male odor than female odor, but the low-dose TPhP treatment group lost the preference for male odor, indicating a possible outcome of early life TPhP exposure on sexual recognition. In the sexual behavior test, both the EE and TPhP treatment groups displayed significantly less proceptive behavior. These results suggest that early life exposure to TPhP disturbs the normal sexual behavior of female rats.

Time series of hexabromocyclododecane transfers from flame-retarded curtains to attached dust.

While the production and new use of hexabromocyclododecane (HBCD) mostly ceased after being listed as a persistent organic pollutant under the Stockholm Convention in 2013, its emission from treated products in use to indoor environments still deserves attention. To examine the transfer of HBCD diastereomers to dust on the surface of flame-retarded curtains and to better characterize the potential of treated fabrics to be sources of HBCD in dust, we carried out a series of 196-day experiments using two types of curtains and attached dusts. Concurrently, the physicochemical properties (vapor pressure, water solubility, and octanol-water partition coefficient) of the HBCD diastereomers were measured. HBCD diastereomers migrated from curtains to dust with half-saturation times of about 20-50 days. By day 196, mean HBCD concentrations in dust had reached 13-290 µg/g, depending on the types of curtains and dusts. The composition of HBCD, dominated by γ-HBCD in the curtains, was dominated by α-HBCD in the post-experiment dusts, probably because of the higher vapor pressure of α-HBCD compared to γ-HBCD. The initial HBCD contents of the two curtains were comparable, but the concentrations and profiles of HBCD diastereomers in the post-experiment dusts differed markedly, probably because differences between the texture and/or surface finishing of the treated fabrics affected HBCD transfer to the attached dust.

Composition and Elution Behavior of Various Elements from Printed Circuit Boards, Cathode-ray Tube Glass, and Liquid-crystal Displays in Waste Consumer Electronics.

The contents and elution behavior of metals in consumer electronics parts were determined so as to understand their maximum environmental risk. Elements contained most in printed-circuit boards were Cu, Si, Br, Ca, Al, Sn, Pb, Sb, Ba, Fe, Ni, Ti, and Zn; in cathode-ray tube glass were Si, Pb, Ba, Sr, Zn, Zr, Ca, and Sb; in arsenic contained liquid-crystal displays were Si, Ca, Sr, Ba, As, and Fe; and in antimony contained liquid-crystal displays were Si, Ba, Ca, Sb, Sr, Fe, and Sn. The elements eluted most from printed-circuit boards were Zn, Pb, and Cu; from cathode-ray tube glass were Pb, Zn, B, Ba, and Si; and from liquid-crystal displays were B and Si, and the toxic As and Sb. The amount eluted was greatest at acidic pH. It was revealed that officially recommended 6-h-shaking with a pure water test was insufficient to understand the real environmental risk of waste electronics.

Effect of lead speciation on its oral bioaccessibility in surface dust and soil of electronic-wastes recycling sites.

We measured bioaccessible lead (Pb) in simulated gastrointestinal fluids containing Pb-contaminated soil or dust from electronic waste (e-waste) recycling sites to assess the risk of Pb ingestion. The physiologically based extraction test (PBET) was used as in vitro bioaccessibility assay. Pb speciation was determined using X-ray absorption spectroscopy. The total Pb concentrations in dusts (n=8) and soils (n=4) were in the range of 1630-131,000 and 239-7800mg/kg, respectively. Metallic Pb, a common component of e-waste, was ubiquitous in the samples. We also found Pb adsorbed onto goethite and as oxides and carbonate, implying soil mixing and weathering influences. Pb phosphate and organic species were only found in the soil samples, suggesting that formation was soil-specific. We identified other Pb compounds in several samples, including Pb silicate, Pb chromate, and Pb(II) hydrogen phosphate. A correlation analysis indicated that metallic Pb decreased bioaccessibility in the stomach, while a Pb speciation analysis revealed a low bioaccessibility for Pb phosphates and high bioaccessibility for organic Pb species. The health risk based on bioaccessible Pb was estimated to be much lower than that of total Pb due to the lower concentrations.

Early-life exposure to Tris(1,3-dichloroisopropyl) phosphate induces dose-dependent suppression of sexual behavior in male rats.

Exposure to endocrine-disrupting chemicals may adversely affect animals, particularly during development. Tris(1,3-dichloroisopropyl) phosphate (TDCIPP) is an organophosphate with anti-androgen function in vitro that is present in indoor dust at relatively high concentrations. In male rats, androgens are necessary for the development of reproductive organs, as well as the endocrine and central nervous systems. However, we currently do not know the exact effects of TDCIPP exposure through suckling on subsequent reproductive behavior in males. Here, we show that TDCIPP exposure (25-250 mg kg-1 via oral administration over 28 consecutive days post-birth) suppressed male sexual behavior and reduced testes size. These changes were dose-dependent and appeared first in adults rather than in juveniles. These results demonstrate that TDCIPP exposure led to normal body growth and appearance in juveniles, but disrupted the endocrine system and physiology in adults. Therefore, assays should be performed using adult animals to ensure accuracy, and to confirm the influence of chemical substances given during early mammalian life.

Exposure assessment of heavy metals in an e-waste processing area in northern Vietnam.

In developing countries, inappropriate recycling of e-waste has resulted in the environmental release of toxicants, including heavy metals, that may have deleterious health effects. In this study, we estimated daily metal intakes in five households in a Vietnamese village located in an e-waste processing area and assessed the health risk posed by exposure to the metals. Garden soil, floor dust, 24-h duplicate diet, and ambient air samples were collected from five households in northern Vietnam in January 2014. All samples were acid-digested, and contents of Cd, Cu, Mn, Pb, Sb, and Zn were measured by using ICP mass spectrometry and ICP atomic emission spectroscopy. In addition, the soil, dust, and diet samples were subjected to an bioaccessibility extraction test to determine bioaccessible metal concentrations. Hazard quotients were estimated from bioaccessible metal concentrations, provisional tolerable weekly intakes, and reference doses. Garden soil and floor dust were estimated to be mainly contributors to daily Pb intake, as indicated by calculations using bioaccessible metal concentrations and the U.S. Environmental Protection Agency soil plus dust ingestion rate. Diet was suggested to contribute significantly to daily Cd, Cu, Mn, Sb, and Zn intake. Estimated metal exposures via inhalation were negligible, as indicated by calculations using International Atomic Energy Agency reference inhalation rates. The maximum hazard quotients were calculated as 0.2 (Cd), 0.09 (Cu), 0.3 (Mn), 0.6 (Pb), 0.2 (Sb), and 0.5 (Zn), on the basis of bioaccessible metal concentrations. The contributions of Cd, Cu, Mn, Sb, and Zn except Pb to potential noncancer risk for adult residents of the five households in the e-waste processing area may be low.

Screening data for the endocrine disrupting activities of 583 chemicals using the yeast two-hybrid assay.

We screened 583 chemicals for receptor binding activity to the human estrogen receptor (hER), the Japanese medaka estrogen receptor (medER), and the aryl hydrocarbon receptor (AhR) using the yeast two-hybrid assay. The substances tested included substances that could potentially be produced unintentionally by industrial processes, such as halogenated steroids and phenols. Antagonistic effects on hER and the androgen receptor were also screened. The test chemicals were selected for screening on the basis of chemical structure associated with possible estrogen receptor binding activity. The current study presents the report on the screening of 583 chemicals for different kinds of endocrine disrupting activity.

Separate screening of brominated and chlorinated dioxins in field samples using in vitro reporter gene assays with rat and mouse hepatoma cell lines.

In 2011, a joint World Health Organization (WHO) and United Nations Environment Programme expert panel recommended the use of the WHO toxicity equivalency factor (TEF) scheme for assessment of the human health risks of brominated dioxins which have different sources from chlorinated dioxins. Therefore, WHO toxic equivalents (TEQs) should be determined for both chlorinated and brominated dioxins. As alternative to the conventional but time-consuming dioxin analysis using gas chromatography high-resolution mass spectrometry, we have developed a screening method involving cleanup and separation of brominated dioxins from chlorinated dioxins in field samples and subsequent analysis by CALUX (chemically activated luciferase expression) assays which are in vitro reporter gene assays detecting dioxin-like compounds. Cleanup and separation were accomplished with silica gel columns impregnated with 55% sulfuric acid and with 10% silver nitrate, respectively, and the average recoveries of the major contributors to the WHO-TEQs were approximately 90%. The CALUX 2,3,7,8-TCDD equivalents (CALUX-TEQs) derived from all the dioxin-like compounds in the cleanup fractions of the field samples (n = 24) were measured by means of the CALUX assays, indicating significant positive correlations between the WHO-TEQs and CALUX-TEQs (r ≥ 0.969, P < 0.001). We found that the ratios of the chlorinated dioxin-derived WHO-TEQs to the brominated dioxin-derived WHO-TEQs were strongly positively correlated with the ratios of the CALUX-TEQs derived from the chlorinated dioxin fractions to the CALUX-TEQs derived from the brominated dioxin fractions (r ≥ 0.833, P < 0.001). These results suggest that our method will be useful for estimating the contributions of chlorinated and brominated dioxins to WHO-TEQs.

Occurrence, profiles, and toxic equivalents of chlorinated and brominated polycyclic aromatic hydrocarbons in E-waste open burning soils.

We conducted this study to assess the occurrence, profiles, and toxicity of chlorinated polycyclic aromatic hydrocarbons (Cl-PAHs) and brominated polycyclic aromatic hydrocarbons (Br-PAHs) in e-waste open burning soils (EOBS). In this study, concentrations of 15 PAHs, 26 Cl-PAHs and 14 Br-PAHs were analyzed in EOBS samples. We found that e-waste open burning is an important emission source of Cl-PAHs and Br-PAHs as well as PAHs. Concentrations of total Cl-PAHs and Br-PAHs in e-waste open burning soil samples ranged from 21 to 2800 ng/g and from 5.8 to 520 ng/g, respectively. Compared with previous studies, the mean of total Cl-PAH concentrations of the EOBS samples in this study was higher than that of electronic shredder waste, that of bottom ash, and comparable to fly ash from waste incinerators in Korea and Japan. The mean of total Br-PAH concentrations of the EOBS samples was generally three to four orders of magnitude higher than those in incinerator bottom ash and comparable to incinerator fly ash, although the number of Br-PAH congeners measured differed among studies. We also found that the Cl-PAH and Br-PAH profiles were similar among all e-waste open burning soil samples but differed from those in waste incinerator fly ash. The profiles and principal component analysis results suggested a unique mechanism of Cl-PAH and Br-PAH formation in EOBS. In addition, the Cl-PAHs and Br-PAHs showed high toxicities equivalent to PCDD/Fs measured in same EOBS samples when calculated based on their relative potencies to benzo[a]pyrene. Along with chlorinated and brominated dioxins and PAHs, Cl-PAHs and Br-PAHs are important environmental pollutants to investigate in EOBS.

Concentrations of polybrominated diphenyl ethers and alternative flame retardants in surface soils and river sediments from an electronic waste-processing area in northern Vietnam, 2012-2014.

We investigated the concentrations of polybrominated diphenyl ethers (PBDEs) and alternative flame retardants (FRs) in environmental samples collected in January 2012, 2013, and 2014 from an electronic waste-processing area in northern Vietnam. During the study period, PBDE and alternative FR concentrations in soils around the electronic waste-processing workshops ranged from 37 to 9200 ng g-1 dry weight (dw) and from 35 to 24,000 ng g-1 dw; the concentrations in soils around the open-burning sites ranged from 1.6 to 62 ng g-1 dw and from <4 to 1900 ng g-1 dw; and the concentrations in river sediments around the workshops ranged from 100 to 3800 ng g-1 dw and from 23 to 6800 ng g-1 dw, respectively. Over the course of study period, we observed significant decreases in concentrations of PBDEs and significant increases in concentrations of alternative FRs, particularly Dechlorane Plus isomers and oligomeric organophosphorus FRs (o-PFRs) in both soils and sediments around the workshops. We also report information on concentrations and environmental emissions of o-PFRs and their low-molecular-weight impurities in the same soils and sediments. The detection of o-PFR impurities around the workshops and the open-burning sites highlights an enhanced breakdown of o-PFRs probably due to weathering during open storage and high temperature attained during the burning of electronic wastes.

Dioxin-like activities, halogenated flame retardants, organophosphate esters and chlorinated paraffins in dust from Australia, the United Kingdom, Canada, Sweden and China.

The concentrations of organic flame retardants (FRs) and dioxin-like activities in dust collected from five countries were investigated. The correlations between the concentrations of the different groups of FRs and dioxin-like activities were examined. Chlorinated paraffins (CPs, C9 to C31) were found in the highest concentration (median ∑CP 700 µg/g, range 280-4750 µg/g), followed by organophosphate esters (median ∑13OPEs 56 µg/g, range 21-110 µg/g), halogenated flame retardants (median ∑17HFRs 3.3 µg/g, range 0.87-14 µg/g) and polybrominated diphenyl ethers (median ∑17PBDEs 2.8 µg/g, range 0.46-11 µg/g). There were no significant differences in concentrations of the FRs among the countries but differences in PBDE and CP congener profiles were found. BDE209 predominated in dust from Australia, the UK, Sweden and China, ranging from 50 to 70% of total PBDEs. The lowest percentage of BDE209 was found in the dust from Canada, representing only 20% of total PBDEs. For CPs in dust from Sweden, the long-chain CPs (especially C18 congeners) predominated, while for other countries, medium-chain CPs (especially C14 congeners) predominated. The dioxin-activities of the dusts ranged from 58 to 590 pg CALUX-TEQ/g, and had a median of 200 pg CALUX-TEQ/g. There were significant positive correlations between concentrations of PBDEs and CPs with dioxin-like activities. The dioxin-like activity may be due to the presence of polychlorinated or polybrominated dioxin/furans (PBDD/DFs) or polychlorinated naphthalenes (PCNs) in the dust. The PBDD/DFs are known impurities and degradation product of the penta-BDE mixture, and PCNs are known impurities of CPs which exhibit dioxin-like activities.

Emerging halogenated flame retardants and hexabromocyclododecanes in food samples from an e-waste processing area in Vietnam.

This study reports concentrations of selected emerging halogenated flame retardants (HFRs) and hexabromocyclododecanes (HBCDs) in foodstuffs sourced from an e-waste processing area in Vietnam and two reference sites in Vietnam and Japan. Concentrations of all target HFRs in e-waste-impacted samples in this study exceed significantly (p < 0.05) those detected in the controls, suggesting that e-waste processing activities exert a substantial impact on local environmental contamination and human dietary exposure. Significant linear positive correlations in concentrations of syn-Dechlorane Plus (DP) and anti-DP were found between soils and those in co-located chicken samples (p < 0.05). This implies that soil is an important exposure source of DPs in chickens at our sampling sites. The estimated dietary intakes of emerging HFRs in this study were 170 and 420 ng per kg bw per day for adults and children, respectively, while daily ingestions of HBCDs were estimated to be 480 and 1500 ng per kg bw per day for adults and children, respectively. Exposure at the site monitored in this study exceeds substantially the estimates of dietary exposure to HBCDs in e-waste processing sites and non-e-waste processing areas elsewhere.

Direct contact between dust and HBCD-treated fabrics is an important pathway of source-to-dust transfer.

Hexabromocyclododecanes (HBCDs) are a class of brominated flame retardant that have found extensive application in consumer products used widely in indoor environments. Although uncertainty remains about the human health impacts of HBCDs, ingestion of HBCD-contaminated indoor dust has been shown to be a particularly significant exposure pathway for young children. Despite this, understanding of the mechanisms via which HBCD transfer from products to indoor dust remains incomplete. In this study, an in-house test chamber was used to investigate transfer of HBCDs from a treated textile sample to indoor dust via direct textile:dust contact. Results were compared with previous data using the same test chamber to examine other pathways via which HBCDs transfer from products to dust, and highlighted HBCD transfer via direct source:dust contact as being particularly important. This novel finding was corroborated by complementary experiments that examined HBCD transfer via direct contact, from other treated textiles to three major components of indoor dust: artificial indoor dust, soil particles, and cotton linters.

Leaching behaviour of hexabromocyclododecane from treated curtains.

A series of laboratory experiments were conducted, whereby two HBCDD treated polyester curtain samples were contacted with deionised Milli-Q water as leaching fluid and HBCDD determined in the resulting leachate. As well as single batch (no replenishment of leaching fluid), serial batch (draining of leachate and replenishment with fresh leaching fluid at various time intervals) experiments were conducted. In single batch experiments at 20 °C, ΣHBCDD concentrations increased only slightly with increasing contact time (6 h, 24 h, and 48 h). This is supported by serial batch tests at 20 °C in which leaching fluid was replaced after 6 h, 24 h, 48 h, 72 h, 96 h, and 168 h. Data from these experiments show that while concentrations of HBCDD in leachate after 24 h cumulative contact time exceed those at 6 h; concentrations in samples collected at subsequent contact times remained steady at ∼50% of those in the 24 h sample. Consistent with this, leaching is shown to be second order, whereby a period of initially intense dissolution of more labile HBCDD is followed by a slower stage corresponding to external diffusion of the soluble residue within the textile. In experiments conducted at 20 °C, α-HBCDD is preferentially leached compared to ß- and γ-HBCDD. However, at higher temperatures, the relatively more hydrophobic diastereomers are proportionally more readily leached, i.e. raising the temperature from 20 °C to 80 °C increased concentrations of γ-HBCDD in the leachate by a factor of 28-33 while corresponding α-HBCDD concentrations only increased by a factor of 4.3-4.8.

Compositional Analysis of Commercial Oligomeric Organophosphorus Flame Retardants Used as Alternatives for PBDEs: Concentrations and Potential Environmental Emissions of Oligomers and Impurities.

Four commercial oligomeric organophosphorus flame retardants (o-PFRs) were characterized using a refractive index detector and atmospheric pressure photoionization (APPI)-quadrupole time-of-flight mass spectrometry (QTOF-MS) compatible with gel permeation chromatography (GPC). Commercial o-PFRs consisted of approximately 90% or more oligomers and several impurities. Triphenyl phosphate (TPHP), tris(dimethylphenyl) phosphate (TDMPP), tris(2-chloroisopropyl) phosphate (TCIPP), and some new impurities were identified as byproducts of some manufacturing process of commercial o-PFRs for the first time. The concentrations of TPHP, TDMPP, and TCIPP were more than 1 weight %, whereas those of new impurities might be approximately 1 weight % by comparison among their abundances acquired through GPC-APPI-QTOF-MS analysis. Based on their vapor pressure and water solubility estimations, the potential environmental emissions of low molecular weight impurities were expected to be higher than those of oligomers. The presence and environmental emissions of low molecular weight impurities might be regarded as risk factors along with commercial o-PFRs.

Comprehensive characterisation of flame retardants in textile furnishings by ambient high resolution mass spectrometry, gas chromatography-mass spectrometry and environmental forensic microscopy.

The presence and levels of flame retardants (FRs), such as polybrominated diphenyl ethers (PBDEs) and organophosphate flame retardants (PFRs), was determined in textile home furnishings, such as carpets and curtains from stores in Belgium. A comprehensive characterisation of FRs in textile was done by ambient high resolution mass spectrometry (qualitative screening), gas chromatography-mass spectrometry (GC-MS) (quantitation), and environmental forensic microscopy (surface distribution). Ambient ionisation coupled to a time-of-flight (TOF) high resolution mass spectrometer (direct probe-TOF-MS) was investigated for the rapid screening of FRs. Direct probe-TOF-MS proved to be useful for a first screening step of textiles to detect FRs below the levels required to impart flame retardancy and to reduce, in this way, the number of samples for further quantitative analysis. Samples were analysed by GC-MS to confirm the results obtained by ambient mass spectrometry and to obtain quantitative information. The levels of PBDEs and PFRs were typically too low to impart flame retardancy. Only high levels of BDE-209 (11-18% by weight) were discovered and investigated in localised hotspots by employing forensic microscopy techniques. Most of the samples were made of polymeric materials known to be inherently flame retarded to some extent, so it is likely that other alternative and halogen-free FR treatments/solutions are preferred for the textiles on the Belgian market.

Toxic Identification and Evaluation of Androgen Receptor Antagonistic Activities in Acid-Treated Liver Extracts of High-Trophic Level Wild Animals from Japan.

Sulfuric acid-treated liver extracts of representative high-trophic level Japanese animals were analyzed by toxic identification and evaluation (TIE) with chemically activated luciferase expression (CALUX) and chemical analysis to elucidate androgen receptor (AR) antagonistic activities and potential contributions of organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs). The activities were detected in striped dolphins (n = 5), Stejneger's beaked whales (n = 6), golden eagle (n = 1), and Steller's sea eagle (n = 1) with CALUX-flutamide equivalents (FluEQs) as follow: 38 (20-52), 47 (21-96), 5.0, and 80 µg FluEQ/g-lipid, respectively. The AR antagonism was detected in limited number of specimens at lower levels for finless porpoise, raccoon dog, and common cormorant. Theoretical activities (Theo-FluEQs) were calculated using the concentration of OCPs and PCBs and their IC25-based relative potency (REP) values. These total contribution to CALUX-FluEQ was 126%, 84%, 53%, 55%, and 44% for striped dolphin, Steller's sea eagle, Stejneger's beaked whale, finless porpoise, and golden eagle, respectively, and the main contributor was p,p'-DDE. However, most of the activities for raccoon dog (7.6%) and common cormorant (17%) could not be explained by OCPs and PCBs. This suggests other unknown compounds could function as AR antagonists in these terrestrial species.