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1.
Nature ; 600(7889): 456-461, 2021 12.
Artículo en Inglés | MEDLINE | ID: mdl-34912090

RESUMEN

Commercial chemicals are used extensively across urban centres worldwide1, posing a potential exposure risk to 4.2 billion people2. Harmful chemicals are often assessed on the basis of their environmental persistence, accumulation in biological organisms and toxic properties, under international and national initiatives such as the Stockholm Convention3. However, existing regulatory frameworks rely largely upon knowledge of the properties of the parent chemicals, with minimal consideration given to the products of their transformation in the atmosphere. This is mainly due to a dearth of experimental data, as identifying transformation products in complex mixtures of airborne chemicals is an immense analytical challenge4. Here we develop a new framework-combining laboratory and field experiments, advanced techniques for screening suspect chemicals, and in silico modelling-to assess the risks of airborne chemicals, while accounting for atmospheric chemical reactions. By applying this framework to organophosphate flame retardants, as representative chemicals of emerging concern5, we find that their transformation products are globally distributed across 18 megacities, representing a previously unrecognized exposure risk for the world's urban populations. More importantly, individual transformation products can be more toxic and up to an order-of-magnitude more persistent than the parent chemicals, such that the overall risks associated with the mixture of transformation products are also higher than those of the parent flame retardants. Together our results highlight the need to consider atmospheric transformations when assessing the risks of commercial chemicals.


Asunto(s)
Contaminantes Atmosféricos/efectos adversos , Contaminantes Atmosféricos/análisis , Atmósfera/química , Monitoreo del Ambiente , Retardadores de Llama/efectos adversos , Sustancias Peligrosas/análisis , Internacionalidad , Organofosfatos/efectos adversos , Aire/análisis , Contaminantes Atmosféricos/química , Contaminantes Atmosféricos/envenenamiento , Animales , Bioacumulación , Ciudades/estadística & datos numéricos , Simulación por Computador , Ecosistema , Retardadores de Llama/análisis , Retardadores de Llama/envenenamiento , Sustancias Peligrosas/efectos adversos , Sustancias Peligrosas/química , Sustancias Peligrosas/envenenamiento , Humanos , Intoxicación por Organofosfatos , Organofosfatos/análisis , Organofosfatos/química , Medición de Riesgo
2.
Anal Chem ; 96(12): 4942-4951, 2024 Mar 26.
Artículo en Inglés | MEDLINE | ID: mdl-38478960

RESUMEN

Bromochloro alkanes (BCAs) have been manufactured for use as flame retardants for decades, and preliminary environmental risk screening suggests they are likely to behave similarly to polychlorinated alkanes (PCAs), subclasses of which are restricted as Stockholm Convention Persistent Organic Pollutants (POPs). BCAs have rarely been studied in the environment, although some evidence suggests they may migrate from treated-consumer materials into indoor dust, resulting in human exposure via inadvertent ingestion. In this study, BCA-C14 mixture standards were synthesized and used to validate an analytical method. This method relies on chloride-enhanced liquid chromatography-electrospray ionization-Orbitrap-high resolution mass spectrometry (LC-ESI-Orbitrap-HRMS) and a novel CP-Seeker integration software package for homologue detection and integration. Dust sample preparation via ultrasonic extraction, acidified silica cleanup, and fractionation on neutral silica cartridges was found to be suitable for BCAs, with absolute recovery of individual homologues averaging 66 to 78% and coefficients of variation ≤10% in replicated spiking experiments (n = 3). In addition, a total of 59 indoor dust samples from six countries, including Australia (n = 10), Belgium (n = 10), Colombia (n = 10), Japan (n = 10), Thailand (n = 10), and the United States of America (n = 9), were analyzed for BCAs. BCAs were detected in seven samples from the U.S.A., with carbon chain lengths of C8, C10, C12, C14, C16, C18, C24 to C28, C30 and C31 observed overall, though not detected in samples from any other countries. Bromine numbers of detected homologues in the indoor dust samples ranged Br1-4 as well as Br7, while chlorine numbers ranged Cl2-11. BCA-C18 was the most frequently detected, observed in each of the U.S.A. samples, while the most prevalent degrees of halogenation were homologues of Br2 and Cl4-5. Broad estimations of BCA concentrations in the dust samples indicated that levels may approach those of other flame retardants in at least some instances. These findings suggest that development of quantification strategies and further investigation of environmental occurrence and health implications are needed.


Asunto(s)
Contaminación del Aire Interior , Retardadores de Llama , Humanos , Monitoreo del Ambiente , Organofosfatos/análisis , Polvo/análisis , Retardadores de Llama/análisis , Contaminación del Aire Interior/análisis , Halógenos , Dióxido de Silicio/análisis
3.
Environ Sci Technol ; 58(20): 8825-8834, 2024 May 21.
Artículo en Inglés | MEDLINE | ID: mdl-38712863

RESUMEN

Flame retardants (FRs) are added to vehicles to meet flammability standards, such as US Federal Motor Vehicle Safety Standard FMVSS 302. However, an understanding of which FRs are being used, sources in the vehicle, and implications for human exposure is lacking. US participants (n = 101) owning a vehicle of model year 2015 or newer hung a silicone passive sampler on their rearview mirror for 7 days. Fifty-one of 101 participants collected a foam sample from a vehicle seat. Organophosphate esters (OPEs) were the most frequently detected FR class in the passive samplers. Among these, tris(1-chloro-isopropyl) phosphate (TCIPP) had a 99% detection frequency and was measured at levels ranging from 0.2 to 11,600 ng/g of sampler. TCIPP was also the dominant FR detected in the vehicle seat foam. Sampler FR concentrations were significantly correlated with average ambient temperature and were 2-5 times higher in the summer compared to winter. The presence of TCIPP in foam resulted in ∼4 times higher median air sampler concentrations in winter and ∼9 times higher in summer. These results suggest that FRs used in vehicle interiors, such as in seat foam, are a source of OPE exposure, which is increased in warmer temperatures.


Asunto(s)
Retardadores de Llama , Retardadores de Llama/análisis , Humanos , Temperatura , Exposición a Riesgos Ambientales , Vehículos a Motor
4.
Environ Sci Technol ; 58(11): 4937-4947, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38446036

RESUMEN

Bis(2-ethylhexyl)-tetrabromophthalate (TBPH), a typical novel brominated flame retardant, has been ubiquitously identified in various environmental and biotic media. Consequently, there is an urgent need for precise risk assessment based on a comprehensive understanding of internal exposure and the corresponding toxic effects on specific tissues. In this study, we first investigated the toxicokinetic characteristics of TBPH in different tissues using the classical pseudo-first-order toxicokinetic model. We found that TBPH was prone to accumulate in the liver rather than in the gonad, brain, and muscle of both female and male zebrafish, highlighting a higher internal exposure risk for the liver. Furthermore, long-term exposure to TBPH at environmentally relevant concentrations led to increased visceral fat accumulation, signaling potential abnormal liver function. Hepatic transcriptome analysis predominantly implicated glycolipid metabolism pathways. However, alterations in the profile of associated genes and biochemical indicators revealed gender-specific responses following TBPH exposure. Besides, histopathological observations as well as the inflammatory response in the liver confirmed the development of nonalcoholic fatty liver disease, particularly in male zebrafish. Altogether, our findings highlight a higher internal exposure risk for the liver, enhancing our understanding of the gender-specific metabolic-disrupting potential associated with TBPH exposure.


Asunto(s)
Retardadores de Llama , Pez Cebra , Animales , Masculino , Femenino , Hígado/metabolismo , Metabolismo de los Lípidos , Retardadores de Llama/toxicidad , Retardadores de Llama/análisis
5.
Environ Sci Technol ; 58(9): 4381-4391, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38381810

RESUMEN

Organophosphate diesters (di-OPEs), as additives in industrial applications and/or transformation products of emerging environmental pollutants, such as organophosphate triesters (tri-OPEs), have been found in the environment and biological matrices. The metabolic fate of di-OPEs in biological media is of great significance for tracing the inherent and precursor toxicity variations. This is the first study to investigate the metabolism of a suite of di-OPEs by liver microsomes and to identify any metabolite of metabolizable di-OPEs in in vitro and in vivo samples. Of the 14 di-OPEs, 5 are significantly metabolizable, and their abundant metabolites with hydroxyl, carboxyl, dealkylated, carbonyl, and/or epoxide groups are tentatively identified. More than half of the di-OPEs are detectable in human serum and/or wild fish tissues, and dibenzyl phosphate (DBzP), bis(2,3-dibromopropyl) phosphate (BDBPP), and isopropyl diphenyl phosphate (ip-DPHP) are first reported at a detectable level in humans and wildlife. Using an in vitro assay and a known biotransformation rule-based integrated screening strategy, 2 and 10 suspected metabolite peaks of DEHP are found in human serum and wild fish samples, respectively, and are then identified as phase I and phase II metabolites of DEHP. This study provides a novel insight into fate and persistence of di-OPE and confirms the presence of di-OPE metabolites in humans and wildlife.


Asunto(s)
Dietilhexil Ftalato , Retardadores de Llama , Animales , Humanos , Organofosfatos , Retardadores de Llama/análisis , Ésteres , Biotransformación , Fosfatos , China , Monitoreo del Ambiente
6.
Environ Sci Technol ; 58(5): 2434-2445, 2024 Feb 06.
Artículo en Inglés | MEDLINE | ID: mdl-38265760

RESUMEN

Source characteristics and health risks of indoor organophosphate esters (OPEs) are limited by the lack of knowledge on emission processes. This study attempted to integrate the contents and emissions of OPEs from indoor building materials to assess human health effects. Thirteen OPEs were investigated in 80 pieces of six categories of building materials. OPEs are ubiquitous in the building materials and ∑13OPE contents varied significantly (p < 0.05) from 72.8 ng/g (seam agent) to 109,900 ng/g (wallpaper). Emission characteristics of OPEs from the building materials were examined based on a microchamber method. Depending on the sample category, the observed initial area-specific emission rates of ∑13OPEs varied from 154 ng/m2/h (carpet) to 2760 ng/m2/h (wooden floorboard). Moreover, the emission rate model was developed to predict the release levels of individual OPEs, quantify source contributions, and assess associated exposure risks. Source apportionments of indoor OPEs exhibited heterogeneities in multiple environmental media. The joint OPE contribution of wallpaper and wooden floorboard to indoor dust was up to 94.8%, while latex paint and wooden floorboard were the main OPE contributors to indoor air (54.2%) and surface (76.1%), respectively. Risk assessment showed that the carcinogenic risks of tris(2-chloroethyl) phosphate (3.35 × 10-7) were close to the acceptable level (1 × 10-6) and deserved special attention.


Asunto(s)
Monitoreo del Ambiente , Retardadores de Llama , Humanos , Ésteres/análisis , Retardadores de Llama/análisis , China , Organofosfatos/análisis , Polvo/análisis , Materiales de Construcción
7.
Environ Sci Technol ; 58(9): 4237-4246, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38386008

RESUMEN

Concentrations of polybrominated diphenyl ethers, hexabromocyclododecane (HBCDD), and novel brominated flame retardants (NBFRs) were measured in indoor dust, indoor air, and outdoor air in Birmingham, UK. Concentrations of ΣBFRs ranged from 490 to 89,000 ng/g, 46-14,000 pg/m3, and 22-11,000 pg/m3, respectively, in UK indoor dust, indoor air, and outdoor air. BDE-209 and decabromodiphenyl ethane (DBDPE) were the main contributors. The maximum concentration of DBDPE (10,000 pg/m3) in outdoor air is the highest reported anywhere to date. In contrast with previous studies of outdoor air in Birmingham, we observed significant correlations between concentrations of tri- to hepta-BDEs and HBCDD and temperature. This may suggest that primary emissions from ongoing use of these BFRs have diminished and that secondary emissions (e.g., evaporation from soil) are now a potentially major source of these BFRs in outdoor air. Conversely, the lack of significant correlations between temperature and concentrations of BDE-209 and DBDPE may indicate that ongoing primary emissions from indoor sources remain important for these BFRs. Further research to clarify the relative importance of primary and secondary sources of BFRs to outdoor air is required. Comparison with earlier studies in Birmingham reveals significant (p < 0.05) declines in concentrations of legacy BFRs, but significant increases for NBFRs over the past decade. While there appear minimal health burdens from BFR exposure for UK adults, dust ingestion of BDE-209 may pose a significant risk for UK toddlers.


Asunto(s)
Contaminación del Aire Interior , Retardadores de Llama , Hidrocarburos Bromados , Adulto , Humanos , Contaminación del Aire Interior/análisis , Polvo/análisis , Monitoreo del Ambiente , Retardadores de Llama/análisis , Éteres Difenilos Halogenados/análisis , Reino Unido , Bromo/análisis
8.
Environ Sci Technol ; 58(15): 6804-6813, 2024 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-38512799

RESUMEN

The pervasive contamination of novel brominated flame retardants (NBFRs) in remote polar ecosystems has attracted great attention in recent research. However, understanding regarding the trophic transfer behavior of NBFRs in the Arctic and Antarctic marine food webs is limited. In this study, we examined the occurrence and trophodynamics of NBFRs in polar benthic marine sediment and food webs collected from areas around the Chinese Arctic Yellow River Station (n = 57) and Antarctic Great Wall Station (n = 94). ∑7NBFR concentrations were in the range of 1.27-7.47 ng/g lipid weight (lw) and 0.09-1.56 ng/g lw in the Arctic and Antarctic marine biota, respectively, among which decabromodiphenyl ethane (DBDPE) was the predominant compound in all sample types. The biota-sediment bioaccumulation factors (g total organic carbon/g lipid) of NBFRs in the Arctic (0.85-3.40) were 4-fold higher than those in the Antarctica (0.13-0.61). Trophic magnification factors (TMFs) and their 95% confidence interval (95% CI) of individual NBFRs ranged from 0.43 (95% CI: 0.32, 0.60) to 1.32 (0.92, 1.89) and from 0.34 (0.24, 0.49) to 0.92 (0.56, 1.51) in the Arctic and Antarctic marine food webs, respectively. The TMFs of most congeners were significantly lower than 1, indicating a trophic dilution potential. This is one of the very few investigations on the trophic transfer of NBFRs in remote Arctic and Antarctic marine ecosystems, which provides a basis for exploring the ecological risks of NBFRs in polar regions.


Asunto(s)
Retardadores de Llama , Regiones Antárticas , Retardadores de Llama/análisis , Cadena Alimentaria , Ecosistema , Bioacumulación , Regiones Árticas , Monitoreo del Ambiente , Lípidos , Éteres Difenilos Halogenados/análisis
9.
Environ Sci Technol ; 58(11): 4904-4913, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38437168

RESUMEN

The Yangtze River fishery resources have declined strongly over the past few decades. One suspected reason for the decline in fishery productivity, including silver carp (Hypophthalmichthys molitrix), has been linked to organophosphate esters (OPEs) contaminant exposure. In this study, the adverse effect of OPEs on lipid metabolism in silver carp captured from the Yangtze River was examined, and our results indicated that muscle concentrations of the OPEs were positively associated with serum cholesterol and total lipid levels. In vivo laboratory results revealed that exposure to environmental concentrations of OPEs significantly increased the concentrations of triglyceride, cholesterol, and total lipid levels. Lipidome analysis further confirmed the lipid metabolism dysfunction induced by OPEs, and glycerophospholipids and sphingolipids were the most affected lipids. Hepatic transcriptomic analysis found that OPEs caused significant alterations in the transcription of genes involved in lipid metabolism. Pathways associated with lipid homeostasis, including the peroxisome proliferator-activated receptor (PPAR) signal pathway, cholesterol metabolism, fatty acid biosynthesis, and steroid biosynthesis, were significantly changed. Furthermore, the affinities of OPEs were different, but the 11 OPEs tested could bind with PPARγ, suggesting that OPEs could disrupt lipid metabolism by interacting with PPARγ. Overall, this study highlighted the harmful effects of OPEs on wild fish and provided mechanistic insights into OPE-induced metabolic disorders.


Asunto(s)
Carpas , Retardadores de Llama , Enfermedades Metabólicas , Animales , Ríos , PPAR gamma , Ésteres/análisis , Organofosfatos/toxicidad , Organofosfatos/análisis , Colesterol/análisis , Lípidos , Retardadores de Llama/análisis , China , Monitoreo del Ambiente/métodos
10.
Environ Sci Technol ; 58(18): 7986-7997, 2024 May 07.
Artículo en Inglés | MEDLINE | ID: mdl-38657129

RESUMEN

The indoor environment is a typical source for organophosphorus flame retardants and plasticizers (OPFRs), yet the source characteristics of OPFRs in different microenvironments remain less clear. This study collected 109 indoor air samples and 34 paired indoor dust samples from 4 typical microenvironments within a university in Tianjin, China, including the dormitory, office, library, and information center. 29 target OPFRs were analyzed, and novel organophosphorus compounds (NOPs) were identified by fragment-based nontarget analysis. Target OPFRs exhibited the highest air and dust concentrations of 46.2-234 ng/m3 and 20.4-76.0 µg/g, respectively, in the information center, where chlorinated OPFRs were dominant. Triphenyl phosphate (TPHP) was the primary OPFR in office air, while tris(2-chloroethyl) phosphate dominated in the dust. TPHP was predominant in the library. Triethyl phosphate (TEP) was ubiquitous in the dormitory, and tris(2-butoxyethyl) phosphate was particularly high in the dust. 9 of 25 NOPs were identified for the first time, mainly from the information center and office, such as bis(chloropropyl) 2,3-dichloropropyl phosphate. Diphenyl phosphinic acid, two hydroxylated and methylated metabolites of tris(2,4-ditert-butylphenyl) phosphite (AO168), and a dimer phosphate were newly reported in the indoor environment. NOPs were widely associated with target OPFRs, and their human exposure risk and environmental behaviors warrant further study.


Asunto(s)
Contaminación del Aire Interior , Polvo , Retardadores de Llama , Compuestos Organofosforados , Plastificantes , Retardadores de Llama/análisis , Plastificantes/análisis , Contaminación del Aire Interior/análisis , Polvo/análisis , China , Compuestos Organofosforados/análisis , Monitoreo del Ambiente , Humanos , Contaminantes Atmosféricos/análisis
11.
Environ Sci Technol ; 58(9): 4368-4380, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38386007

RESUMEN

Despite the increasing health risks shown by the continuous detection of organophosphate esters (OPEs) in biota in recent years, information on the occurrence and potential risks of OPEs in marine mammals remains limited. This study conducted the first investigation into the body burdens and potential risks of 10 traditional OPEs (tOPEs) and five emerging OPEs (eOPEs) in 10 cetacean species (n = 84) from the northern South China Sea (NSCS) during 2005-2021. All OPEs, except for 2-ethylhexyl diphenyl phosphate (EHDPHP), were detected in these cetaceans, indicating their widespread occurrence in the NSCS. Although the levels of the ∑10tOPEs in humpback dolphins remained stable from 2005 to 2021, the concentrations of the ∑5eOPEs showed a significant increase, suggesting a growing demand for these new-generation OPEs in South China. Dolphins in proximity to urban regions generally exhibited higher OPE concentrations than those from rural areas, mirroring the environmental trends of OPEs occurring in this area. All OPE congeners, except for EHDPHP, in humpback dolphins exhibited a maternal transfer ratio >1, indicating that the dolphin placenta may not be an efficient barrier for OPEs. The observed significant correlations between levels of OPEs and hormones (triiodothyronine, thyroxine, and testosterone) in humpback dolphins indicated that OPE exposures might have endocrine disruption effects on the dolphin population.


Asunto(s)
Delfines , Retardadores de Llama , Animales , Monitoreo del Ambiente , Bioacumulación , Ésteres , China , Organofosfatos , Fosfatos , Retardadores de Llama/análisis
12.
Anal Bioanal Chem ; 416(6): 1493-1504, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38280016

RESUMEN

Organophosphate flame retardants (OPFRs) are high-production volume chemicals widely present in environmental compartments. The presence of water-soluble OPFRs (tri-n-butyl phosphate (TnBP), tris(2-butoxyethyl) phosphate (TBEP), tris(2-chloroethyl) phosphate (TCEP), tris(2-chloroisopropyl) phosphate (TCPP), and triethyl phosphate (TEP)) in water compartments evidences the struggle of conventional wastewater treatment plants (WWTPs) to effectively eliminate these toxic compounds. This study reports for the first time the use of white-rot fungi as a promising alternative for the removal of these OPFRs. To accomplish this, a simple and cost-efficient quantification method for rapid monitoring of these contaminants' concentrations by GC-MS while accounting for matrix effects was developed. The method proved to be valid and reliable for all the tested parameters. Sample stability was examined under various storage conditions, showing the original samples to be stable after 60 days of freezing, while post-extraction storage techniques were also effective. Finally, a screening of fungal degraders while assessing the influence of the glucose regime on OPFR removal was performed. Longer chain organophosphate flame retardants, TBP and TBEP, could be easily and completely removed by the fungus Ganoderma lucidum after only 4 days. This fungus also stood out as the sole organism capable of partially degrading TCEP (35% removal). The other chlorinated compound, TCPP, was more easily degraded and 70% of its main isomer was removed by T. versicolor. However, chlorinated compounds were only partially degraded under nutrient-limiting conditions. TEP was either not degraded or poorly degraded, and it is likely that it is a transformation product from another OPFR's degradation. These results suggest that degradation of chlorinated compounds is dependent on the concentration of the main carbon source and that more polar OPFRs are less susceptible to degradation, given that they are less accessible to radical removal by fungi. Overall, the findings of the present study pave the way for further planned research and a potential application for the degradation of these contaminants in real wastewaters.


Asunto(s)
Retardadores de Llama , Compuestos Organofosforados , Fosfinas , Compuestos Organofosforados/análisis , Retardadores de Llama/análisis , Cromatografía de Gases y Espectrometría de Masas , Organofosfatos/análisis , Aguas Residuales , Agua , Fosfatos
13.
Environ Res ; 248: 118308, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38281563

RESUMEN

Despite numerous data on organophosphate tri-esters (tri-OPEs) in the environment, literatures on organophosphate di-esters (di-OPEs) in field environment, especially marine sediments remain scarce. This study addresses this gap by analyzing 35 abyssal sediment samples from the middle Okinawa Trough in the East China Sea. A total of 25 tri-OPEs and 10 di-OPEs were determined, but 13 tri-OPEs and 2 di-OPEs were nondetectable in any of these sediment samples. The concentrations of ∑12tri-OPE and ∑8di-OPE were 0.108-32.2 ng/g (median 1.11 ng/g) and 0.548-15.0 ng/g (median 2.74 ng/g). Chlorinated (Cl) tri-OPEs were the dominant tri-esters, accounting for 47.5 % of total tri-OPEs on average, whereas chlorinated di-OPEs represented only 19.2 % of total di-OPEs. This discrepancy between the relatively higher percentage of Cl-tri-OPEs and lower abundance of Cl-di-OPEs may be ascribed to the stronger environmental persistence of chlorinated tri-OPEs. Source assessment suggested that di-OPEs were primarily originated from the degradation of tri-OPEs rather than industrial production. Long range waterborne transport facilitated by oceanic currents was an important input pathway for OPEs in sediments from the Okinawa Trough. These findings enhance the understanding of the sources and transport of OPEs in marine sediments, particularly in the Okinawa Trough.


Asunto(s)
Monitoreo del Ambiente , Retardadores de Llama , Ésteres , Retardadores de Llama/análisis , China , Organofosfatos , Sedimentos Geológicos
14.
Environ Res ; 248: 118223, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38286254

RESUMEN

Dust is a sink for flame retardants, which are added to a myriad of consumer products in residential spaces. Organophosphate esters (OPEs) and brominated flame retardants (BFRs) are two classes of flame retardants that are frequently used in consumer products and consequently found in dust. In this present work, a novel solvent-limited microextraction technique, which we detailed in a companion study, was applied for the determination of four OPEs and two BFRs with limits of quantitation at the ng/g level by gas chromatography-mass spectrometry and liquid chromatography-mass spectrometry from n = 47 air filter dust samples collected from forced air HVAC systems. Levels of the BFRs, including tetrabromobisphenol-A and its derivative tribromobisphenol-A, were found at levels <4 µg/g and not frequently detected. Conversely, all four OPEs were detected in all air filter dust samples. Total OPE load was dominated by tris(2,4-di-tert-butylphenyl) phosphate, T24DtBPP, a novel OPE not widely examined in the literature. Comparison of individual and total OPE concentrations to residential characteristics revealed statistically significant relationships to location of the home and dominant flooring type. Overall, this study motivates future work in examining the whole house exposome using air filter dust as a passive sampling regime with more examination of T24DtBPP loads within other indoor spaces.


Asunto(s)
Filtros de Aire , Contaminación del Aire Interior , Exposoma , Retardadores de Llama , Retardadores de Llama/análisis , Polvo/análisis , Organofosfatos/análisis , Contaminación del Aire Interior/análisis , Monitoreo del Ambiente , Ésteres/análisis
15.
Environ Res ; 251(Pt 1): 118614, 2024 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-38462084

RESUMEN

Organophosphate esters (OPEs) have been widely used as flame retardants and plasticizers in consumer and industrial products. They have been found to have numerous exposure hazards. Recently, several OPEs have been detected in surface waters around the world, which may pose potential ecological risks to freshwater organisms. In this study, the concentration, spatial variation, and ecological risk of 15 OPEs in the Beiyun and Yongding rivers were unprecedentedly investigated by the ultra-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) and risk quotient (RQ) method. The result showed that triethyl phosphate (TEP), tri (2-chloroisopropyl) phosphate (TCPP) were the most abundant OPEs with average concentrations of 55.53 ng/L and 42.29 ng/L, respectively. The concentrations of OPEs in the Beiyun River are higher than in the Yongding River, and their levels were higher in densely populated and industrial areas. The risk assessment showed that there was insignificant from OPEs to freshwater organisms in these rivers (RQs <0.1). The risk was higher downstream than upstream, which was related to human-intensive industrial activities downstream in the Yongding River. The ecological risk of OPEs in surface waters worldwide was estimated by joint probability curves (JPCs), and the result showed that there was a moderate risk for tri (2-chloroethyl) phosphate (TCEP), a low risk for trimethyl phosphate (TMP), and insignificant for other OPEs. In addition, the QSAR-ICE-SSD model was used to calculate the hazardous concentration for 5% (HC5). This result validated the feasibility and accuracy of this model in predicting acute data of OPEs and reducing biological experiments on the toxicity of OPEs. These results revealed the ecological risk of OPEs and provided the scientific basis for environmental managers.


Asunto(s)
Monitoreo del Ambiente , Organofosfatos , Ríos , Contaminantes Químicos del Agua , Medición de Riesgo , Contaminantes Químicos del Agua/análisis , Organofosfatos/análisis , Ríos/química , Ésteres/análisis , China , Espectrometría de Masas en Tándem , Retardadores de Llama/análisis , Ciudades
16.
Environ Res ; 251(Pt 1): 118580, 2024 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-38423496

RESUMEN

BACKGROUND AND AIMS: Exposure to brominated flame retardants (BFRs) has been widely confirmed to impair the normal functioning of the human body system. However, there is a paucity of study on the effects of serum BFRs on bone mineral density (BMD). This study aims to investigate the relationship between exposure to BFRs and BMD in a nationally representative sample of U.S. adults. METHODS: 3079 participants aged between 20 and 80 years with complete data were included in the study. Serum levels of BFRs were measured using automated liquid-liquid extraction and subsequent sample clean-up. The BMD of all participants were assessed by DXA examinations. Generalize linear model, Restricted cubic spline (RCS), subgroup, weighted quantile sum (WQS) and bayesian kernel machine regression (BKMR) were used to estimate the association between serum BFRs and BMD. RESULTS: Multivariate linear regression analyses revealed that, after adjusting for covariates, PBB153 was significantly associated with TF-BMD (ß = 0.0177, 95%CI: 0.0103-0.0252), FN-BMD (ß = 0.009, 95%CI: 0.0036-0.0145), TS-BMD (ß = 0.0081, 95%CI: 0.0013-0.015) and L1-BMD (ß = 0.0144, 95%CI: 0.0075-0.0213). However, the associations lose their statistical significance after further adjustment for sex. BFRs exhibited S-shaped or line-plateau dose-response curves with BMD. In subgroup analyses, BFRs were significantly associated with BMD in participants who were younger than 55 years, female, overweight (BMI >25 kg/m2), and less alcohol consumption. In WQS and BKMR analyses, the effects of BFRs mixtures on BMD differed by sex, and PBDE153, PBDE209 and PBB153 had the highest weights in the WQS regression model. CONCLUSION: This study showed that serum BFRs negatively predicted BMD in men, but not in women or the general population. PBDE153, PBDE209, and PBB153 were significant BMD factors, especially in younger, overweight, and less alcohol consumption individuals.


Asunto(s)
Densidad Ósea , Retardadores de Llama , Encuestas Nutricionales , Humanos , Persona de Mediana Edad , Adulto , Retardadores de Llama/análisis , Femenino , Masculino , Densidad Ósea/efectos de los fármacos , Estudios Transversales , Anciano , Estados Unidos , Adulto Joven , Anciano de 80 o más Años , Exposición a Riesgos Ambientales/efectos adversos , Contaminantes Ambientales/sangre
17.
Environ Res ; 252(Pt 3): 118981, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38663667

RESUMEN

BACKGROUND: Polybrominated diphenyl ethers (PBDEs) are ubiquitous environmental chemicals used as flame retardants in commercial and consumer products. Gestational PBDE concentrations are associated with adverse behaviors in children; however, the persistence of these associations into adolescence remains understudied. OBJECTIVE: We estimated the association of gestational PBDE serum concentrations with early adolescent self- and caregiver-reported behaviors at age 12 years and determined the consistency with previously observed associations in childhood with caregiver-reported behaviors in a prospective pregnancy and birth cohort. METHODS: We measured maternal serum concentrations of five individual PBDE congeners and created a summary exposure variable (∑5BDE: 28, -47, -99, -100 and -153) during pregnancy. At age 12 years, we assessed behaviors for 237 adolescents using self- and caregiver-reports with the Behavioral Assessment System for Children-3 (BASC3). We used multivariable linear regression models to estimate covariate-adjusted associations of lipid standardized, log10-transformed gestational PBDE concentrations with BASC3 scores. We obtained estimates and 95% confidence intervals through a bootstrapping approach. We evaluated potential effect measure modification (EMM) of adolescent sex by examining sex-stratified regression models and estimating the EMM p-values. RESULTS: Gestational PBDE concentrations were positively associated with adolescent-reported BASC3 composite indices for inattention & hyperactivity (BDE-28, -47, -99, -100, ∑5BDE), internalizing problems (BDE-28, -47, -99), functional impairment (BDE-28, ∑5BDE), and emotional symptoms (BDE-28). Gestational PBDE concentrations were positively associated with caregiver-reported BASC3 composite indices for externalizing problems (BDE-28, -47, -99, -100, -153, ∑5BDE) and behavioral symptoms (BDE-99). For caregiver reported behaviors, we observed stronger associations with gestational BDE concentrations among males, especially for executive functioning (BDE-28, -47, -99, -100, ∑5BDE). DISCUSSION: Gestational PBDE serum concentrations were associated with self-reported internalizing and externalizing behavior problems in early adolescence. Caregiver-reported externalizing behaviors recognized during childhood remain associated with gestational PBDE concentrations and persist into early adolescence. Internalizing behaviors were less recognized by caregivers.


Asunto(s)
Contaminantes Ambientales , Éteres Difenilos Halogenados , Efectos Tardíos de la Exposición Prenatal , Humanos , Femenino , Embarazo , Éteres Difenilos Halogenados/sangre , Adolescente , Masculino , Niño , Contaminantes Ambientales/sangre , Efectos Tardíos de la Exposición Prenatal/sangre , Retardadores de Llama/análisis , Estudios Prospectivos , Exposición Materna/efectos adversos , Conducta del Adolescente/psicología
18.
Environ Res ; 250: 118465, 2024 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-38367839

RESUMEN

Estuaries in South Africa are very important for biodiversity conservation and serve as focal points for leisure and tourism activities. The organophosphate flame retardants (OPFRs) levels in these aquatic systems haven't been documented in any studies as of yet. Due to the negative effects of persistent organic pollutants in South African estuaries, we examined the occurrence of eight OPFRs in sediments of two estuaries by studying their spatiotemporal distribution, season variation, and ecological risks. The Sundays Estuary (SDE), a semi-urbanized agricultural surrounding system, recorded an ∑8OPFR concentration in sediments that ranged from 0.71 to 22.5 ng/g dw, whereas Swartkops Estuary, a largely urbanized system, recorded a concentration that ranged from 0.61 to 119 ng/g dw. Alkyl-OPFRs were the prevalent homologue in both estuaries compared to the chlorinated and aryl groups. While TBP, TCPP, and TCrP were the most abundant compounds among the homologue groups. There was no distinct seasonal trend of ∑8OPFR concentration in either estuary, with summer and autumn seasons recording the highest concentrations in SDE and SWE, respectively. Ecological risks in the majority of the study sites for the detected compounds were at low (RQ < 0.1) and medium levels (0.1 ≤ RQ < 1) for certain species of fish, Daphnia magna and algae. However, the cumulative RQs for all the compounds had ∑RQs ≥1 for most sites in both estuaries, indicating that these organisms, if present in both estuaries, may be exposed to potential ecological concerns due to accumulated OPFR chemicals. The scope of future studies should be broadened to include research areas that are not only focus on the bioaccumulation patterns of these compounds but also find sustainable ways to reduce them from these estuarine environments.


Asunto(s)
Monitoreo del Ambiente , Estuarios , Retardadores de Llama , Sedimentos Geológicos , Estaciones del Año , Contaminantes Químicos del Agua , Sedimentos Geológicos/química , Sedimentos Geológicos/análisis , Contaminantes Químicos del Agua/análisis , Sudáfrica , Medición de Riesgo , Retardadores de Llama/análisis , Organofosfatos/análisis , Organofosfatos/toxicidad , Animales
19.
Environ Health ; 23(1): 64, 2024 Jul 13.
Artículo en Inglés | MEDLINE | ID: mdl-39003460

RESUMEN

BACKGROUND: Brominated Flame Retardants (BFRs) have attracted widespread concern due to their environmental persistence and potential toxicity. This study aims to examine the association between BFRs exposure and hypertension. METHODS: We used data from the National Health and Nutrition Examination Survey (NHANES) spanning 2005 to 2016 for the cross-sectional analysis. To evaluate the individual and combined impacts of BFRs exposure on hypertension, we utilized multivariate models, including generalized additive models, weighted quantile sum (WQS) regression, and Bayesian kernel machine regression (BKMR) models. RESULTS: 9882 individuals (48% male) aged ≥ 20 were included in the final analysis, of whom 4114 had hypertension. After controlling for potential covariates, higher serum concentrations of PBDE100 (OR: 1.26; 95% CI: 1.01, 1.57) and PBDE153 (OR: 1.50; 95% CI: 1.18, 1.88) were significantly associated with hypertension. A nonlinear relationship between PBDE28 and hypertension was observed (P = 0.03). Moreover, BFRs mixture were positively associated with the prevalence of hypertension in both the WQS (ß:1.09; 95% CI: 1.02, 1.17; P = 0.02) and BKMR models. CONCLUSION: Our study suggested that BFRs exposure is positively associated with hypertension in the general population. To confirm this association and elucidate the mechanisms, further research is required.


Asunto(s)
Exposición a Riesgos Ambientales , Contaminantes Ambientales , Retardadores de Llama , Éteres Difenilos Halogenados , Hipertensión , Encuestas Nutricionales , Humanos , Retardadores de Llama/análisis , Femenino , Masculino , Hipertensión/epidemiología , Hipertensión/inducido químicamente , Adulto , Persona de Mediana Edad , Éteres Difenilos Halogenados/sangre , Estudios Transversales , Exposición a Riesgos Ambientales/efectos adversos , Contaminantes Ambientales/sangre , Estados Unidos/epidemiología , Adulto Joven , Anciano , Bifenilos Polibrominados/sangre
20.
Gen Comp Endocrinol ; 350: 114469, 2024 05 01.
Artículo en Inglés | MEDLINE | ID: mdl-38360373

RESUMEN

Tetrabromobisphenol A bis(2-hydroxyethyl) ether (TBBPA-DHEE) is the major TBBPA derivative. It has been detected in different environmental samples. Previous studies show that TBBPA-DHEE caused neurotoxicity in rats. In this study, juvenile zebrafish were exposed to various concentrations of TBBPA-DHEE to ascertain the potential neurotoxicity of TBBPA-DHEE, the chemical, and its possible molecular mechanism of action. Behavioral analysis revealed that TBBPA-DHEE could significantly increase the swimming distance and speed in the 1.5 mg/L group compared to the control. In contrast, the swimming distance and speed were significantly reduced in the 0.05 and 0.3 mg/L groups, affecting learning, memory, and neurodevelopment. Similarly, TBBPA-DHEE exposure caused a concentration-dependent significant increase in the levels of excitatory neurotransmitters, namely, dopamine, norepinephrine, and epinephrine, which could be attributed to the change observed in zebrafish behavior. This demonstrates the neurotoxicity of TBBPA-DHEE on juvenile zebrafish. The concentration-dependent increase in the IBR value revealed by the IBR index reveals the noticeable neurotoxic effect of TBBPA-DHEE. Transcriptomic analysis shows that TBBPA-DHEE exposure activated the PPAR signaling pathways, resulting in a disturbance of fatty acid (FA) metabolism and changes in the transcript levels of genes involved in these pathways, which could lead to lipotoxicity and hepatotoxicity. Our findings demonstrate a distinct endocrine-disrupting response to TBBPA-DHEE exposure, possibly contributing to abnormal behavioral alterations. This study provides novel insights into underlying the mechanisms and effects of TBBPA-DHEE on aquatic organisms, which may be helpful forenvironmental/human health risk assessments of the emerging pollutant.


Asunto(s)
Retardadores de Llama , Pez Cebra , Humanos , Ratas , Animales , Pez Cebra/metabolismo , Éteres/análisis , Éteres/metabolismo , Análisis de Secuencia de ARN , Retardadores de Llama/toxicidad , Retardadores de Llama/análisis , Retardadores de Llama/metabolismo
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