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1.
Anal Chem ; 2021 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-33845572

RESUMO

Ion mobility mass spectrometry (IM-MS)-derived collision cross section (CCS) values can serve as a valuable additional identification parameter within the analysis of compounds of emerging concern (CEC) in human matrices. This study introduces the first comprehensive database of DTCCSN2 values of 148 CECs and their metabolites including bisphenols, alternative plasticizers (AP), organophosphate flame retardants (OP), perfluoroalkyl chemicals (PFAS), and others. A total of 311 ions were included in the database, whereby the DTCCSN2 values for 113 compounds are reported for the first time. For 105 compounds, more than one ion is reported. Moreover, the DTCCSN2 values of several isomeric CECs and their metabolites are reported to allow a distinction between isomers. Comprehensive quality assurance guidelines were implemented in the workflow of acquiring DTCCSN2 values to ensure reproducible experimental conditions. The reliability and reproducibility of the complied database were investigated by analyzing pooled human urine spiked with 30 AP and OP metabolites at two concentration levels. For all investigated metabolites, the DTCCSN2 values measured in urine showed a percent error of <1% in comparison to database values. DTCCSN2 values of OP metabolites showed an average percent error of 0.12% (50 ng/mL in urine) and 0.15% (20 ng/mL in urine). For AP metabolites, these values were 0.10 and 0.09%, respectively. These results show that the provided database can be of great value for enhanced identification of CECs in environmental and human matrices, which can advance future suspect screening studies on CECs.

2.
Environ Int ; 153: 106540, 2021 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-33838618

RESUMO

The COVID-19 outbreak has forced countries to introduce severe restrictive measures to contain its spread. In particular, physical distancing and restriction of movement have had important consequences on human behaviour and potentially also on illicit drug use and supply. These changes can be associated with additional risks for users, in particular due to reduced access to prevention and harm reduction activities. Furthermore, there have been limitations in the amount of data about drug use which can be collected due to restrictions. To goal of this study was to obtain information about potential changes in illicit drug use impacted by COVID-19 restrictions. Wastewater samples were collected in seven cities in the Netherlands, Belgium, Spain and Italy at the beginning of lockdowns (March-May 2020). Using previously established and validated methods, levels of amphetamine (AMP), methamphetamine (METH), MDMA, benzoylecgonine (BE, the main metabolite of cocaine) and 11-nor-9-carboxy-Δ9-tetrahydrocannabinol (THC-COOH, main metabolite of tetrahydrocannabinol (THC)) were measured and compared with findings from previous years. Important differences in levels of consumed drugs were observed across the considered countries. Whilst for some substances and locations, marked decreases in consumption could be observed (e.g., 50% decrease in MDMA levels compared to previous years). In some cases, similar or even higher levels compared to previous years could be found. Changes in weekly patterns were also observed, however these were not clearly defined for all locations and/or substances. Findings confirm that the current situation is highly heterogeneous and that it remains very difficult to explain and/or predict the effect that the present pandemic has on illicit drug use and availability. However, given the current difficulty in obtaining data due to restrictions, wastewater analysis can provide relevant information about the situation at the local level, which would be hard to obtain otherwise.

3.
Toxics ; 9(4)2021 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-33800558

RESUMO

Communicating individual human biomonitoring results to study participants has been the subject of debate for some time. This debate is dominated by ethical considerations from a researchers' perspective on whether or not to communicate, thereby overlooking more practice-based questions from a participants' perspective on what and how to communicate. We conducted a small scale follow-up study based on eleven face-to-face interviews with mothers participating in the third cycle of the Flemish Environment and Health Study (FLEHS III 2012-2015) to investigate how they experienced and interpreted individual biomonitoring results. Key findings indicate that respondents were generally satisfied with participating in the biomonitoring study, but the report-back process especially lacked contextualized information and interactive communication options to better comprehend and cope with personal results. These findings also argue in favor of a more tailored approach in which report-back methods, formats and content are diversified according to the type of results and the preferences of participants. A reflexive research practice with active engagement in follow-up research is crucial to improve participants' understanding and use of personal biomonitoring results.

4.
Environ Int ; 152: 106511, 2021 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-33773387

RESUMO

BACKGROUND: Chemicals of Emerging Concern (CECs) include a very wide group of chemicals that are suspected to be responsible for adverse effects on health, but for which very limited information is available. Chromatographic techniques coupled with high-resolution mass spectrometry (HRMS) can be used for non-targeted screening and detection of CECs, by using comprehensive annotation databases. Establishing a database focused on the annotation of CECs in human samples will provide new insight into the distribution and extent of exposures to a wide range of CECs in humans. OBJECTIVES: This study describes an approach for the aggregation and curation of an annotation database (CECscreen) for the identification of CECs in human biological samples. METHODS: The approach consists of three main parts. First, CECs compound lists from various sources were aggregated and duplications and inorganic compounds were removed. Subsequently, the list was curated by standardization of structures to create "MS-ready" and "QSAR-ready" SMILES, as well as calculation of exact masses (monoisotopic and adducts) and molecular formulas. The second step included the simulation of Phase I metabolites. The third and final step included the calculation of QSAR predictions related to physicochemical properties, environmental fate, toxicity and Absorption, Distribution, Metabolism, Excretion (ADME) processes and the retrieval of information from the US EPA CompTox Chemicals Dashboard. RESULTS: All CECscreen database and property files are publicly available (DOI: https://doi.org/10.5281/zenodo.3956586). In total, 145,284 entries were aggregated from various CECs data sources. After elimination of duplicates and curation, the pipeline produced 70,397 unique "MS-ready" structures and 66,071 unique QSAR-ready structures, corresponding with 69,526 CAS numbers. Simulation of Phase I metabolites resulted in 306,279 unique metabolites. QSAR predictions could be performed for 64,684 of the QSAR-ready structures, whereas information was retrieved from the CompTox Chemicals Dashboard for 59,739 CAS numbers out of 69,526 inquiries. CECscreen is incorporated in the in silico fragmentation approach MetFrag. DISCUSSION: The CECscreen database can be used to prioritize annotation of CECs measured in non-targeted HRMS, facilitating the large-scale detection of CECs in human samples for exposome research. Large-scale detection of CECs can be further improved by integrating the present database with resources that contain CECs (metabolites) and meta-data measurements, further expansion towards in silico and experimental (e.g., MassBank) generation of MS/MS spectra, and development of bioinformatics approaches capable of using correlation patterns in the measured chemical features.

5.
Sci Total Environ ; 777: 145914, 2021 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-33677284

RESUMO

WBE was applied to evaluate illicit drug (i.e. amphetamine, cocaine, MDMA and methamphetamine), alcohol and tobacco use in three Lithuanian cities in 2018 and 2019. Considerable concentrations of methamphetamine and MDMA were found in the three locations, suggesting a specific Lithuanian consumption pattern. Yet, unexpected high concentrations of amphetamine (>4 µg/L) were detected in two samples of Kaunas in 2018. Through the use of chiral analysis and non-target and suspect drug precursor compound screening, these extreme values were confirmed to be the result of direct disposal of amphetamine in the sewers. Furthermore, substantial alcohol use was measured in the three investigated catchment populations of Lithuania with almost 4 standard drinks/day/inhabitant aged 15+ on average in 2019. For tobacco, an average of 5.6 cigarettes/day/inhabitant aged 15+ in 2019 was reported with large discrepancies between WBE figures and sales data, potentially highlighting illegal trade of tobacco products.

6.
Sci Total Environ ; 770: 145346, 2021 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-33736417

RESUMO

Exposure to certain perfluoroalkyl acids (PFAAs) can have considerable effects on the endocrine and immune systems, although such effects remain largely uncharacterized in wildlife. Using an apex avian predator, we investigated possible relationships of thyroid hormones (THs), specifically free (F) and total (T) thyroxine (FT4; TT4) and triiodothyronine (FT3; TT3), and the expression of an immune-related microRNA biomarker (i.e., miR-155), with the concentrations of 11 PFAAs in nestling peregrine falcons (Falco peregrinus). Nestling peregrines (n = 56; usually two chicks of each sex per nest) were blood sampled when 23 ± 4 days old in urban and rural regions of the Laurentian Great Lakes Basin (Ontario, Canada) in 2016 and 2018. The circulating concentrations of several PFAAs were significantly associated with THs and estimated thyroid gland activity (TT3:TT4; FT3:FT4), including PFHxS (FT3; FT3:FT4), PFDS (TT3; TT3:TT4), PFOA (TT4; FT3:FT4), PFTeDA (TT4; FT3:FT4), PFHxDA (TT4; TT3:TT4) and ΣPFCAs (TT4). Our novel evaluation of miR-155 in peregrine nestlings identified significantly negative relationships of plasma miR-155 counts with PFHxS and PFOA concentrations, indicating potential down-regulation of miR-155 expression and impaired immunity. Several PFAA homologues significantly predicted the variation in THs and miR-155 in conjunction with year (e.g., inter-annual differences in weather, ambient temperature, rainfall), region (urban/rural), nestling age, and/or diet (trophic position; δ15N), which suggests that multiple environmental and biological stressors, including PFAA exposure, influenced thyroid activity and immune function in these nestlings. Further research is warranted to identify the mechanisms and additional impacts of PFAA-related thyroid and immune disruption on the growth, development, and health risks in developing birds.


Assuntos
Falconiformes , Fluorcarbonetos , MicroRNAs , Animais , Fluorcarbonetos/toxicidade , Ontário , Hormônios Tireóideos , Tiroxina , Tri-Iodotironina
7.
Artigo em Inglês | MEDLINE | ID: mdl-33530429

RESUMO

This study investigates the presence of Stockholm Convention listed short-chain chlorinated paraffins (SCCPs) and their replacement medium-chain chlorinated paraffins (MCCPs) counterparts in polyvinyl chloride and rubber consumer products and toys purchased on the Belgian market in 2019. SCCPs were detected in 27/28 samples at concentrations ranging from

Assuntos
Hidrocarbonetos Clorados , Parafina , Bélgica , China , Monitoramento Ambiental , Hidrocarbonetos Clorados/análise , Parafina/análise , Cloreto de Polivinila , Borracha
8.
Environ Pollut ; 276: 116724, 2021 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-33631684

RESUMO

Restrictions on the use of legacy phthalate esters (PEs) as plasticizer chemicals in several consumer products has led to the increased use of alternative plasticizers (APs), such as di-(iso-nonyl)-cyclohexane-1,2-dicarboxylate (DINCH) and di-(2-ethylhexyl) terephthalate (DEHTP). In the fourth cycle of the Flemish Environment and Health Study (FLEHS IV, 2016-2020), we monitored exposure to seven PEs (diethyl phthalate (DEP), di-(2-ethylhexyl) phthalate (DEHP), di-isobutyl phthalate (DiBP), di-n-butyl phthalate (DnBP), butylbenzyl phthalate (BBzP, di-isononyl phthalate (DINP), and di-isodecyl phthalate (DIDP))and three APs (DINCH, DEHTP, and di-(2-ethylhexyl) adipate (DEHA)) by measuring multiple biomarkers in urine of 416 adolescents from Flanders, Belgium (14-15 years old). The reference values show that exposure to PEs is still widespread, although levels of several PE metabolites (e.g., sum of DEHP metabolites, mono-normal-butyl phthalate (MnBP) and mono-benzyl phthalate (MBzP)) have decreased significantly compared to previous human biomonitoring cycles (2003-2018). On the other hand, metabolites of DINCH and DEHTP were detected in practically every participant. Concentrations of AP exposure biomarkers in urine were generally lower than PE metabolites, but calculations of estimated daily intakes (EDIs) showed that exposure to DINCH and DEHTP can be considerable. However, preliminary risk assessment showed that none of the EDI or urinary exposure levels of APs exceeded the available health-based guidance values, while a very low number of participants had levels of MiBP and MnBP exceeding the HBM value. Several significant determinants of exposure could be identified from multiple regression models: the presence of building materials containing PVC, ventilation habits, socio-economic status and season were all associated with PE and AP biomarker levels. Cumulatively, the results of FLEHS IV show that adolescents in Flanders, Belgium, are exposed to a wide range of plasticizer chemicals. Close monitoring over the last decade showed that the exposure levels of restricted PEs have decreased, while newer APs are now frequently detected in humans.


Assuntos
Poluentes Ambientais , Ácidos Ftálicos , Adolescente , Bélgica , Biomarcadores , Exposição Ambiental/análise , Humanos , Plastificantes
9.
Environ Pollut ; 277: 116795, 2021 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-33640813

RESUMO

Investigating environmental pollution is important to understand its impact on endangered species such as green turtles (Chelonia mydas). In this study, we investigated the accumulation and potential toxicity of selected persistent organic pollutants (POPs) and naturally occurring MeO-PBDEs in liver, fat, kidney and muscle of turtles (n = 30) of different gender, size, year of death, location and health status. Overall, POP concentrations were low and accumulation was highest in liver and lowest in fat which is likely due to the poor health of several animals, causing a remobilization of lipids and associated compounds. PCBs and p,p'-DDE dominated the POP profiles, and relatively high MeO-PBDE concentrations (2'-MeO-BDE 68 up to 192 ng/g lw, 6-MeO-BDE 47 up to 79 ng/g lw) were detected in all tissues. Only few influences of factors such as age, gender and location were found. While concentrations were low compared to other marine wildlife, biological toxicity equivalences obtained by screening the tissue extracts using the micro-EROD assay ranged from 2.8 to 356 pg/g and the highest values were observed in muscle, followed by kidney and liver. This emphazises that pollutant mixtures found in the turtles have the potential to cause dioxin-like effects in these animals and that dioxin-like compounds should not be overlooked in future studies.


Assuntos
Bifenilos Policlorados , Tartarugas , Poluentes Químicos da Água , Animais , Monitoramento Ambiental , Éteres Difenil Halogenados/toxicidade , Bifenilos Policlorados/toxicidade , Poluentes Químicos da Água/toxicidade
11.
BMC Pediatr ; 21(1): 99, 2021 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-33637059

RESUMO

BACKGROUND: We report data of a Belgian observational prospective cohort study regarding cognitive and behavioural development until the age of 36 months in relation to internal exposure to organochlorine pollutants [sum of polychlorinated biphenyls (sum PCB), dioxin-like activity, PCB118, PCB170, hexachlorobenzene (HCB) and p,p'-dichlorodiphenyldichloroethylene (DDE)] measured in cord blood. METHODS: Participants were recruited as part of an Flemish Environmental Health Survey (2002-2006). Two hundred and six mother-child pairs were recruited. Hundred twenty five toddlers [Reynell Taal Ontwikkelings Schalen (language development, RTOS), Snijders-Oomen Niet-verbale intelligentietest (non-verbal intelligence, SON), Bayley Scales, milestones, Infant Behaviour Questionnaire (IBQ), gender specific play behaviour, Neurobehavioral Evaluation System (NES)-attentional task] and their mothers [Home Observation Measurement of the Environment (HOME), Wechsler Abbreviated Scale of Intelligence (WASI), State-Trait Anxiety Inventory (STAI), general questionnaires] were tested. Statistical analysis was performed with the SPSS program. Much attention was paid to confounding factors. RESULTS: In the first years of development, higher organochlorine pollutants were associated with less active children (delayed crawling: sum PCB*HCB (p < 0.05), sumPCB*DDE (p < 0.1); delayed first steps alone: sum PCB (p < 0.5), PCB118 (p < 0.01), PCB170 (p < 0.01), HCB (p < 0.01); less switching between toys: sum PCB (p < 0.01); less switching between toys in boys: PCB118 (p < 0.01), sum PCB(p < 0.01)). At 12 months children with higher dioxin-like activity tended to show less fear responses(p < 0.1) (IBQ 12 months). At 36 months, a slower development of language comprehension (RTOS) was related to all organochlorine exposure parameters(p < 0.1 or p < 0.05) except DDE. Lower nonverbal IQ scores (SON) were related to PCB118 in boys only(p < 0.05 or p < 0.01). Less masculine and more non-gender specific play behaviour was associated with sum PCB in boys and girls at 36 months(p < 0.1). Moreover, PCB118 (p < 0.05), PCB170 (p < 0.1), HCB(p < 0.05) and DDE(p < 0.05) were associated with diminished masculine play behaviour in boys. CONCLUSION: Our data confirm the observations that neurobehavioral development of young children is adversely influenced by environmental concentrations of PCBs, especially in boys. In this context, observation of play behaviour seems to be a reliable, easy to perform and sensitive test to detect neurotoxic effects of chemicals like PCB's and dioxin-like compounds in very young children. On the basis of our results, we hypothesize that an underarrousal pattern may play a role in the spectrum of effects measured in toddlers prenatally exposed to PCBs and dioxin-like compounds.

12.
Drug Test Anal ; 2021 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-33395730

RESUMO

Phosphatidylethanol 16:0/18:1 (PEth) is the most abundant homologue of the phosphatidylethanol group of phospholipids. Formed only in the presence of ethanol, PEth is used as a biomarker in whole blood to provide information about the consumption of alcohol. As information on the storage life of PEth is essential for its beneficial use as a biomarker, this study investigated the stability of PEth in spiked and authentic whole blood samples stored at 4°C. Human whole blood samples (n = 23) and spiked whole blood samples (n = 7) with a concentration range between 5 and 2000 ng/ml were analysed at specific time intervals, up to 90 days. Differences were evident between the stability of authentic and spiked samples. PEth was stable at 4°C for 60 days (concentrations within 15% of initial concentration) in authentic samples, whereas spiked samples were stable for up to 30 days. This study emphasizes the importance of including authentic samples in stability experiments.

13.
Environ Res ; 195: 110745, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33460637

RESUMO

The widespread occurrence of persistent organic pollutants (POPs) in the environment is a matter of concern. In this study, selected organohalogenated contaminants, including dichlorodiphenyltrichloroethane and its metabolites (DDTs) polychlorinated biphenyls (PCBs), chlordanes (CHLs), hexachlorobenzene (HCB), polybrominated diphenyl ethers (PBDEs), hexabromocyclododecanes (HBCDs), tetrabromobisphenol A (TBBPA), 2,4,6-tribromophenol (TBP), were measured in complete meal sets (24-h duplicate-diet) of Japanese infants to investigate the levels, profiles, and possible sources of contamination. In total, 46 whole-day meals of infants (7-24-months old) were collected during 2017 from Fukuoka, Japan. To the best of our knowledge, this is the first report based on the duplicate-diet method for infants. The median intakes among the POP groups were highest for ΣDDTs (18 ng/day, maximum 251 ng/day), followed by ΣPCBs (17 ng/day, maximum 198 ng/day), ΣCHLs (14 ng/day, maximum 105 ng/day), HCB (11 ng/day, maximum 64 ng/day), TBP (3.5 ng/day, maximum 109 ng/day), ΣHBCDs (1.9 ng/day, maximum 70 ng/day), TBBPA (0.72 ng/day, maximum 34 ng/day), and ΣPBDEs (0.11 ng/day, maximum 4.5 ng/day). Among the PCBs, PCB-138 and PCB-153 were the most abundant congeners (27% and 23%, respectively). p,p'-DDE, the major DDT metabolite, accounted for 96% of total DDTs. Among PBDEs, BDE47 was the only detected congener (present in 4% of the samples). The dietary intake of the targeted compounds was lower than the intake via breast milk, suggesting that the exposure from baby food was limited. In the principal component analysis, chlorinated and brominated compounds were separated on principal component 1, while TBP and α-HBCD were separated on principal component 2, likely suggesting a differing emission time trend or source. PCB-153, PCB-138, trans-chlordane, cis-chlordane, and trans-nonachlor were correlated with seafood consumption (Spearman's ρ = 0.45 to 0.57, p < 0.05), while TBP was correlated with seaweed consumption (Spearman's ρ = 0.46, p < 0.05). Also, four species of commercial edible seaweed in Japan were analyzed to confirm the findings of the duplicate-diet study. The relatively high concentration of TBP (5.5 ± 6.6 ng/g wet weight) was observed in the seaweed samples, indicating that seaweed is a potential exposure source of TBP.

14.
Environ Int ; 147: 106368, 2021 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-33421765

RESUMO

The ubiquitous use of organophosphate flame retardants and plasticizers (PFRs) in a variety of consumer products has led to widespread human exposure. Since certain PFRs are developmental and carcinogenic toxicants, detailed exposure assessments are essential to investigate the risk associated with environmental exposure levels. However, such data are still lacking for European countries. In this study, concentrations of thirteen PFR metabolites were measured in urine samples from 600 adolescents from Flanders, Belgium. 1-Hydroxy-2-propyl bis(1-chloro-2-propyl) phosphate (BCIPHIPP), diphenyl phosphate (DPHP), bis(1,3-dichloro-isopropyl) phosphate (BDCIPP), 2-hydroxyethyl bis(2-butoxyethyl) phosphate (BBOEHEP), 2-ethylhexyl phenyl phosphate (EHPHP) and 2-ethyl-5-hydroxyhexyl diphenyl phosphate (5-HO-EHDPHP) were frequently detected (>83%) in all participants. Comparisons with study populations from outside the EU showed that urinary levels of DPHP, BDCIPP and BCIPHIPP were generally within the same range. Only exposure to 2-ethylhexyl diphenyl phosphate (EHDPHP) was presumably higher in Flemish adolescents. However, determinants analysis through multivariate regression analyses did not reveal significant predictors that may explain this finding. Significantly higher levels of BDCIPP were observed in participants with new decorations at home, while adolescents with highly educated parents had higher levels of BBOEHEP and BDCIPP. Furthermore, multiple PFR metabolite concentrations followed a seasonal pattern. Estimated daily intakes (EDIs) were calculated from the internal dose by including fractions of urinary excretion (FUE) estimated in in vitro metabolism studies. EDIs ranged from 6.3 ng/kg bw/day for TBOEP to 567.7 ng/kg bw/day for EHDPHP, which were well below the available oral reference doses for all investigated PFRs. This suggests that the associated risk is low at present. This is the first report on internal exposure to seven commonly used PFRs in a European population.

15.
Chemosphere ; 263: 127817, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-32841870

RESUMO

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


Assuntos
Poluição do Ar em Ambientes Fechados , Poeira , Poluição do Ar em Ambientes Fechados/análise , Bélgica , Poeira/análise , Espectrometria de Massas , Organofosfatos/análise
16.
J Hazard Mater ; 404(Pt A): 124079, 2021 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-33017711

RESUMO

Bisphenol F (BPF) and bisphenol S (BPS) are becoming widespread in the environment despite the lack of information regarding their fate during wastewater treatment and in the environment. This study assessed the biodegradation kinetics of BPF and BPS during biological wastewater treatment with activated sludge using GC-MS/MS, and the identification of biotransformation products (BTPs) using LC-QTOF-MS. The results showed that BPF and BPS degrade readily and unlikely accumulate in biosolids or wastewater effluent (ci = 0.1 mg L-1, half-lives <4.3 days). The first-order kinetic model revealed that BPF (kt = 0.20-0.38) degraded faster than BPS (kt = 0.04-0.16) and that degradation rate decreases with an increasing initial concentration of BPS (half-lives 17.3 days). The absence of any additional organic carbon source significantly slowed down degradation, in particular, that of BPS (lag phase on day 18 instead of day 7). The machine-learning algorithm adopted as part of the non-targeted workflow identified three known BTPs and one novel BTP of BPF, and one known and ten new BTPs of BPS. The data from this study support possible new biodegradation pathways, namely sulphation, methylation, cleavage and the coupling of smaller bisphenol moieties.

17.
J Chromatogr A ; 1637: 461807, 2021 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-33360078

RESUMO

The analysis of polar metabolites based on liquid chromatography-mass spectrometry (LC-MS) methods should take into consideration the complexity of interactions in LC columns to be able to cover a broad range of metabolites of key biological pathways. Therefore, in this study, different chromatographic columns were tested for polar metabolites including reversed-phase and hydrophilic interaction liquid chromatography (HILIC) columns. Based on a column screening, two new generations of zwitterionic HILIC columns were selected for further evaluation. A tree-based method optimization was applied to investigate the chromatographic factors affecting the retention mechanisms of polar metabolites with zwitterionic stationary phases. The results were evaluated based on a scoring system which was applied for more than 80 polar metabolites with a high coverage of key human metabolic pathways. The final optimized methods showed high complementarity to analyze a wide range of metabolic classes including amino acids, small peptides, sugars, amino sugars, phosphorylated sugars, organic acids, nucleobases, nucleosides, nucleotides and acylcarnitines. Optimized methods were applied to analyze different biological matrices, including human urine, plasma and liver cell extracts using an untargeted approach. The number of high-quality features (< 30% median relative standard deviation) ranged from 3,755 for urine to 5,402 for the intracellular metabolome of liver cells, showing the potential of the methods for untargeted purposes.


Assuntos
Cromatografia Líquida/métodos , Espectrometria de Massas/métodos , Metaboloma , Líquidos Corporais , Humanos , Interações Hidrofóbicas e Hidrofílicas , Metabolômica/métodos , Plasma/química
18.
J Hazard Mater ; 406: 124754, 2021 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-33310325

RESUMO

Organophosphate flame retardants (OPFRs) are substantially applied as flame retardants and plasticizers in consumer products. Although the embryonic developmental toxicity of OPFRs has been reported, human data are limited and the critical windows of susceptibility to OPFRs exposure urgently need to be identified. Here, we investigated the trimester-specific associations between prenatal OPFR exposure and birth size for the first time. The concentrations of 15 OPFR metabolites and tris(2-chloroethyl) phosphate were repeatedly determined in urine samples of 213 pregnant women collected in the first, second, and third trimesters in Wuhan, China, and anthropometric data were retrieved from medical records. In multiple informant models, urinary concentrations of bis(1,3-dichloro-2-propyl) phosphate (BDCIPP) and bis(2-butoxyethyl) phosphate (BBOEP) in the third trimester, 4-hydroxyphenyl-diphenyl phosphate (4-HO-DPHP) in the second trimester, and diphenyl phosphate (DPHP) in the first trimester were negatively associated with birth weight, among which a significant difference in exposure-effect relationships across the three trimesters was observed for BDCIPP. BBOEP concentrations in the third trimester were negatively correlated to birth length with significant varying exposure effects. Our results suggest that prenatal exposure to certain OPFRs may impair fetal growth, and the fetus is vulnerable to the developmental toxicity of BDCIPP and BBOEP in the third trimester.

19.
J Hazard Mater ; 408: 124856, 2021 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-33383451

RESUMO

Neurotoxicity of organophosphate esters (OPEs) has been reported in toxicological studies, but epidemiological findings are limited. We aimed to assess the associations between prenatal OPE exposures and children's neurodevelopment at 2 years old. We measured urinary concentrations of OPEs collected in the first and third trimester from 184 pregnant women in Wuhan, China. Childhood neurodevelopment was assessed using the Chinese revision of Bayley Scale of Infant Development. A two-fold increase in the average of bis (1,3-dichloro-2-propyl) phosphate (BDCIPP) was associated with 3.50 decrease in Psychomotor Development Index (PDI) score (95%CI: -5.86, -1.14) and 5.75 decrease in Mental Development Index (MDI) score (95%CI: -8.94, -2.55). Average of the molar concentrations of chlorinated-alkyl OPEs (ΣCl-OPEs) during pregnancy was inversely associated with PDI [ß = -3.24 (95%CI: -5.95, -0.53)] and MDI scores [ß = -5.86 (95%CI: -9.52, -2.20)]. Prenatal concentrations of BDCIPP and ΣCl-OPEs were inversely associated with neurodevelopment scores in boys, but not in girls. Our study provides evidence that elevated prenatal exposure to chlorinated-alkyl OPEs especially BDCIPP might be inversely associated with childhood neurodevelopment, and the effect seems to be sex-specific.

20.
Environ Res ; 192: 110299, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-33058811

RESUMO

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

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