Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 2.706
Filtrar
Mais filtros

Intervalo de ano de publicação
1.
Nature ; 600(7889): 456-461, 2021 12.
Artigo em Inglês | MEDLINE | ID: mdl-34912090

RESUMO

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.


Assuntos
Poluentes Atmosféricos/efeitos adversos , Poluentes Atmosféricos/análise , Atmosfera/química , Monitoramento Ambiental , Retardadores de Chama/efeitos adversos , Substâncias Perigosas/análise , Internacionalidade , Organofosfatos/efeitos adversos , Ar/análise , Poluentes Atmosféricos/química , Poluentes Atmosféricos/intoxicação , Animais , Bioacumulação , Cidades/estatística & dados numéricos , Simulação por Computador , Ecossistema , Retardadores de Chama/análise , Retardadores de Chama/intoxicação , Substâncias Perigosas/efeitos adversos , Substâncias Perigosas/química , Substâncias Perigosas/intoxicação , Humanos , Intoxicação por Organofosfatos , Organofosfatos/análise , Organofosfatos/química , Medição de Risco
2.
Anal Chem ; 96(12): 4942-4951, 2024 03 26.
Artigo em Inglês | MEDLINE | ID: mdl-38478960

RESUMO

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.


Assuntos
Poluição do Ar em Ambientes Fechados , Retardadores de Chama , Humanos , Monitoramento Ambiental , Organofosfatos/análise , Poeira/análise , Retardadores de Chama/análise , Poluição do Ar em Ambientes Fechados/análise , Halogênios , Dióxido de Silício/análise
3.
Environ Sci Technol ; 58(20): 8825-8834, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38712863

RESUMO

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.


Assuntos
Retardadores de Chama , Retardadores de Chama/análise , Humanos , Temperatura , Exposição Ambiental , Veículos Automotores
4.
Environ Sci Technol ; 58(31): 13613-13623, 2024 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-39051121

RESUMO

China is a significant producer and consumer of various brominated flame retardants (BFRs), raising environmental concerns due to their widespread presence and potential threats to ecosystems and organisms. This study adopts a life cycle perspective, combining material flow analysis, multimedia environmental modeling, and ecological risk assessment to systematically analyze the substance metabolism and ecological risks of six BFR types in China from 1970 to 2021. The findings reveal that China's cumulative BFR consumption reached 3.3 Mt, with the electronics sector being the predominant contributor at 52.1%. Consequently, 1.5 kt of BFRs were released into the environment, with 24.9%, 31.5%, and 43.6% being discharged into the air, water, and soil, respectively. Notably, the proportion of novel BFRs in emissions has steadily increased over the years, exemplified by the increase in decabromodiphenyl ethane (DBDPE) from 21.3% in 2010 to 30.1% in 2021. Geographically, BFR concentrations are higher in the eastern and southwestern regions compared to those in the northwest. Presently, certain BFRs like tetrabromobisphenol A (TBBPA) and DBDPE exhibit moderate to high ecological risks, primarily concentrated in the Shandong and Sichuan provinces. A combination of efficient recycling, emission control, and substitution with novel flame-retardant can minimize the exposure of BFRs to the environment and organisms.


Assuntos
Retardadores de Chama , Retardadores de Chama/análise , China , Medição de Risco , Monitoramento Ambiental
5.
Environ Sci Technol ; 58(11): 4937-4947, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38446036

RESUMO

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.


Assuntos
Retardadores de Chama , Peixe-Zebra , Animais , Masculino , Feminino , Fígado/metabolismo , Metabolismo dos Lipídeos , Retardadores de Chama/toxicidade , Retardadores de Chama/análise
6.
Environ Sci Technol ; 58(9): 4381-4391, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38381810

RESUMO

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.


Assuntos
Dietilexilftalato , Retardadores de Chama , Animais , Humanos , Organofosfatos , Retardadores de Chama/análise , Ésteres , Biotransformação , Fosfatos , China , Monitoramento Ambiental
7.
Environ Sci Technol ; 58(33): 14786-14796, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39106076

RESUMO

In this study, we measured 15 common organophosphate flame retardants (OPFRs) in six categories of tea samples across China. OPFRs were found in all the tea samples, with the total concentrations of OPFRs (∑OPFRs) at 3.44-432 ng/g [geometric mean (GM): 17.6 ng/g]. Triphenyl phosphate (TPhP) was the dominant OPFR, accounting for 39.0-76.2% of ∑OPFRs across all tea categories. The potential factors influencing the residual OPFRs in tea were thoroughly examined, including the agricultural environment, fermentation, and packaging of teas. Tea packaging materials (TPMs) were then identified as the primary sources of OPFRs in teas. The migration test revealed that OPFRs with lower molecular weights and log Kow values exhibited a higher propensity for facilitating the migration of OPFRs from TPMs to teas. The estimated daily intakes of OPFRs from teas were relatively higher for the general populations in Mauritania, Gambia, Togo, Morocco, and Senegal (3.18-9.79 ng/kg bw/day) than China (3.12 ng/kg bw/day). The health risks arising from OPFRs in Chinese teas were minor. This study established a baseline concentration and demonstrated the contamination sources of OPFRs in Chinese tea for the first time, with an emphasis on enhancing the hygiene standards for TPMs.


Assuntos
Retardadores de Chama , Organofosfatos , Chá , Retardadores de Chama/análise , Chá/química , China , Medição de Risco , Embalagem de Alimentos , Humanos , Contaminação de Alimentos
8.
Environ Sci Technol ; 58(9): 4237-4246, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38386008

RESUMO

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.


Assuntos
Poluição do Ar em Ambientes Fechados , Retardadores de Chama , Hidrocarbonetos Bromados , Adulto , Humanos , Poluição do Ar em Ambientes Fechados/análise , Poeira/análise , Monitoramento Ambiental , Retardadores de Chama/análise , Éteres Difenil Halogenados/análise , Reino Unido , Bromo/análise
9.
Environ Sci Technol ; 58(5): 2434-2445, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38265760

RESUMO

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.


Assuntos
Monitoramento Ambiental , Retardadores de Chama , Humanos , Ésteres/análise , Retardadores de Chama/análise , China , Organofosfatos/análise , Poeira/análise , Materiais de Construção
10.
Environ Sci Technol ; 58(15): 6804-6813, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38512799

RESUMO

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.


Assuntos
Retardadores de Chama , Regiões Antárticas , Retardadores de Chama/análise , Cadeia Alimentar , Ecossistema , Bioacumulação , Regiões Árticas , Monitoramento Ambiental , Lipídeos , Éteres Difenil Halogenados/análise
11.
Environ Sci Technol ; 58(9): 4368-4380, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38386007

RESUMO

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.


Assuntos
Golfinhos , Retardadores de Chama , Animais , Monitoramento Ambiental , Bioacumulação , Ésteres , China , Organofosfatos , Fosfatos , Retardadores de Chama/análise
12.
Environ Sci Technol ; 58(11): 4904-4913, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38437168

RESUMO

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.


Assuntos
Carpas , Retardadores de Chama , Doenças Metabólicas , Animais , Rios , PPAR gama , Ésteres/análise , Organofosfatos/toxicidade , Organofosfatos/análise , Colesterol/análise , Lipídeos , Retardadores de Chama/análise , China , Monitoramento Ambiental/métodos
13.
Environ Sci Technol ; 58(18): 7986-7997, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38657129

RESUMO

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.


Assuntos
Poluição do Ar em Ambientes Fechados , Poeira , Retardadores de Chama , Compostos Organofosforados , Plastificantes , Retardadores de Chama/análise , Plastificantes/análise , Poluição do Ar em Ambientes Fechados/análise , Poeira/análise , China , Compostos Organofosforados/análise , Monitoramento Ambiental , Humanos , Poluentes Atmosféricos/análise
14.
Anal Bioanal Chem ; 416(6): 1493-1504, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38280016

RESUMO

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.


Assuntos
Retardadores de Chama , Compostos Organofosforados , Fosfinas , Compostos Organofosforados/análise , Retardadores de Chama/análise , Cromatografia Gasosa-Espectrometria de Massas , Organofosfatos/análise , Águas Residuárias , Água , Fosfatos
15.
Anal Bioanal Chem ; 416(20): 4543-4554, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38877147

RESUMO

Organophosphate flame retardants (OPFRs) are widely used as substitutes for traditional brominated flame retardants, necessitating a reliable and sensitive method for biomonitoring their urinary metabolites to assess human exposure. This study conducted biomonitoring of 10 metabolites of OPFRs in 152 adults and assessed their association with oxidative stress biomarkers 8-hydroxydeoxyguanosine and 8-hydroxyguanosine. Urinary metabolites of OPFRs were released via enzymatic deconjugation. The addition of sodium chloride to the urine samples increases the ionic strength, inducing a salting-out effect that reduces the solubility of these compounds, thereby facilitating their extraction with a mixture of ethyl acetate and acetonitrile. Then, the metabolites of OPFRs were quantified by ultra-high performance liquid chromatography-tandem mass spectrometry, and we validated the method for linear range, precision, matrix effect, and method detection limit. The detection limit of the metabolites of OPFRs ranged from 0.01 to 0.2 µg/L, and these metabolites were detected with high frequencies ranging from 25.0 to 98.68% in the urine samples. The concentration of bis (2-chloroethyl) phosphate was significantly higher in males than in females, with the geometric mean concentration of 0.88 µg/L for males and 0.53 µg/L for females, respectively. Spearman correlation analysis revealed weak but statistically significant positive correlations among the urinary metabolites. Bayesian kernel machine regression analysis showed a significant positive association between elevated urinary concentrations of metabolites of OPFRs and increased oxidative stress levels. Di-n-butyl phosphate was identified as the metabolite that significantly contributed to the elevated level of 8-hydroxyguanosine.


Assuntos
Monitoramento Biológico , Retardadores de Chama , Limite de Detecção , Extração Líquido-Líquido , Compostos Organofosforados , Estresse Oxidativo , Espectrometria de Massas em Tandem , Humanos , Retardadores de Chama/análise , Retardadores de Chama/metabolismo , Espectrometria de Massas em Tandem/métodos , Feminino , Masculino , Cromatografia Líquida de Alta Pressão/métodos , Adulto , Monitoramento Biológico/métodos , Compostos Organofosforados/urina , Extração Líquido-Líquido/métodos , Pessoa de Meia-Idade , Biomarcadores/urina , Adulto Jovem
16.
Macromol Rapid Commun ; 45(14): e2400068, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38593218

RESUMO

With the advantages of lightweight and low thermal conductivity properties, polymeric foams are widely employed as thermal insulation materials for energy-saving buildings but suffer from inherent flammability. Flame-retardant coatings hold great promise for improving the fire safety of these foams without deteriorating the mechanical-physical properties of the foam. In this work, four kinds of sulfur-based flame-retardant copolymers are synthesized via a facile radical copolymerization. The sulfur-containing monomers serve as flame-retardant agents including vinyl sulfonic acid sodium (SPS), ethylene sulfonic acid sodium (VS), and sodium p-styrene sulfonate (VSS). Additionally, 2-hydroxyethyl acrylate (HEA) and 4-hydroxybutyl acrylate are employed to enable a strong interface adhesion with polymeric foams through interfacial H-bonding. By using as-synthesized waterborne flame-retardant polymeric coating with a thickness of 600 µm, the coated polyurethane foam (PUF) can achieve a desired V-0 rating during the vertical burning test with a high limiting oxygen index (LOI) of >31.5 vol%. By comparing these sulfur-containing polymeric fire-retardant coatings, poly(VS-co-HEA) coated PUF demonstrates the best interface adhesion capability and flame-retardant performance, with the lowest peak heat release rate of 166 kW m-2 and the highest LOI of 36.4 vol%. This work provides new avenues for the design and performance optimization of advanced fire-retardant polymeric coatings.


Assuntos
Retardadores de Chama , Polímeros , Poliuretanos , Enxofre , Poliuretanos/química , Polímeros/química , Enxofre/química , Retardadores de Chama/análise , Incêndios
17.
Macromol Rapid Commun ; 45(20): e2400414, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39038120

RESUMO

Carbon fiber (CF)-reinforced epoxy resin (EP) composites are lightweight materials with excellent comprehensive performance. However, the flammability of EP and the poor interfacial bonding between CF and EP are two key disadvantages that limit their further applications. Here, a kind of water-soluble lignin-based CF sizing agent (ELBEDK) is prepared through hydrophilic modification of enzymatic lignin, which can significantly enhance the interfacial interaction between CF and EP. Additionally, a highly efficient intumescent flame retardant (LMA) is prepared. The EP, enzymatic lignin, LMA and CF sized ELBEDK are compounded to obtain the fire-safety CF reinforced composites (SCF/FEP/L). The flame retardancy of SCF/FEP/L with 7% LMA (SCF/FEP7) reached V-0 rating. Moreover, SCF/FEP/L with 7% LMA and 15% lignin (SCF/FEP7/L15) present an limiting oxygen index (LOI)of 30.2% and V-0 of UL-94. Specifically, the total smoke production and the heat release rate are 47.8% and 46.81% lower than that of SCF/EP, respectively, indicating the improved smoke suppression and flame retardancy. The IFSS and flexural strength of SCF/FEP7/L15 are improved to be 59.4 MPa and 511.1 MPa, respectively. This study presents a simple approach to fabricate low-cost high performance lignin-based flame retardant CF/EP biocomposites with wide application potential.


Assuntos
Fibra de Carbono , Resinas Epóxi , Retardadores de Chama , Lignina , Lignina/química , Resinas Epóxi/química , Fibra de Carbono/química , Retardadores de Chama/análise , Incêndios
18.
Environ Res ; 248: 118308, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38281563

RESUMO

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.


Assuntos
Monitoramento Ambiental , Retardadores de Chama , Ésteres , Retardadores de Chama/análise , China , Organofosfatos , Sedimentos Geológicos
19.
Environ Res ; 248: 118223, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38286254

RESUMO

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.


Assuntos
Filtros de Ar , Poluição do Ar em Ambientes Fechados , Expossoma , Retardadores de Chama , Retardadores de Chama/análise , Poeira/análise , Organofosfatos/análise , Poluição do Ar em Ambientes Fechados/análise , Monitoramento Ambiental , Ésteres/análise
20.
Environ Res ; 251(Pt 1): 118580, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38423496

RESUMO

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.


Assuntos
Densidade Óssea , Retardadores de Chama , Inquéritos Nutricionais , Humanos , Pessoa de Meia-Idade , Adulto , Retardadores de Chama/análise , Feminino , Masculino , Densidade Óssea/efeitos dos fármacos , Estudos Transversais , Idoso , Estados Unidos , Adulto Jovem , Idoso de 80 Anos ou mais , Exposição Ambiental/efeitos adversos , Poluentes Ambientais/sangue
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA