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1.
Chemosphere ; 315: 137743, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36608884

RESUMO

This study investigates an electrochemical approach for the treatment of water polluted with per- and poly-fluoroalkyl substances (PFAS), looking at the impact of different variables, contributions from generated radicals, and degradability of different structures of PFAS. Results obtained from a central composite design (CCD) showed the importance of mass transfer, related to the stirring speed, and the amount of charge passed through the electrodes, related to the current density on decomposition rate of PFOA. The CCD informed optimized operating conditions which we then used to study the impact of solution conditions. Acidic condition, high temperature, and low initial concentration of PFOA accelerated the degradation kinetic, while DO had a negligible effect. The impact of electrolyte concentration depended on the initial concentration of PFOA. At low initial PFOA dosage (0.2 mg L-1), the rate constant increased considerably from 0.079 ± 0.001 to 0.259 ± 0.019 min-1 when sulfate increased from 0.1% to 10%, likely due to the production of SO4•-. However, at higher initial PFOA dosage (20 mg L-1), the rate constant decreased slightly from 0.019 ± 0.001 to 0.015 ± 0.000 min-1, possibly due to the occupation of active anode sites by excess amount of sulfate. SO4•- and •OH played important roles in decomposition and defluorination of PFOA, respectively. PFOA oxidation was initiated by one electron transfer to the anode or SO4•-, undergoing Kolbe decarboxylation where yielded perfluoroalkyl radical followed three reaction pathways with •OH, O2 and/or H2O. PFAS electrooxidation depended on the chemical structures where the decomposition rate constants (min-1) were in the order of 6:2 FTCA (0.031) > PFOA (0.019) > GenX (0.013) > PFBA (0.008). PFBA with a shorter chain length and GenX with -CF3 branching had slower decomposition than PFOA. While presence of C-H bonds makes 6:2 FTCA susceptible to the attack of •OH accelerating its decomposition kinetic. Conducting experiments in mixed solution of all studied PFAS and in natural water showed that the co-presence of PFAS and other water constituents (organic and inorganic matters) had adverse effects on PFAS decomposition efficiency.


Assuntos
Fluorcarbonetos , Poluentes Químicos da Água , Fluorcarbonetos/química , Caprilatos/química , Poluentes Químicos da Água/química , Água , Sulfatos/química
2.
Artigo em Inglês | MEDLINE | ID: mdl-36613141

RESUMO

Human milk is the primary source of nutrition for infants in their first year of life. Its potential contamination with perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), a group of toxic man-made chemicals, is a health concern that may threatens infants' health. Our study aims to assess the levels of PFOA and PFOS in the breast milk of Lebanese lactating mothers and the maternal factors associated with their presence. High-performance liquid chromatography (HPLC) coupled with a Micromass Quattro micro API triple quadrupole mass spectrometer was used to detect the level of contamination in 57 collected human milk samples. PFOA and PFOS were present in 82.5% and 85.7% of the samples, respectively, while PFOA levels ranged between 120 and 247 pg/mL with a median of 147 pg/mL, and those of PFOS ranged between 12 and 86 pg/mL with a median of 27.5 pg/mL. The median contamination for PFOA exceeded the threshold set by the European Food Safety Authority (EFSA) (60 pg/mL); however, that of PFOS was below the threshold (73 pg/mL). The consumption of bread, pasta, meat, and chicken more than twice per week and that of white tubers and roots at least once per week was significantly associated with higher levels of PFOA (p < 0.05). No significant association was found between maternal age, BMI, parity, level of education, place of residence, source of water used, and smoking with the levels of PFOA and PFOS in the human milk. Additionally, the consumption of cereals at least twice per week was significantly associated with higher levels of PFOS. These findings call for actions to improve the local environmental and agricultural practices, and the regulations and standards for inspecting imported food. It is important to highlight that the benefits of breastfeeding outweigh the reported contamination with PFOS and PFOA in our study.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Lactente , Gravidez , Feminino , Humanos , Leite Humano/química , Lactação , Líbano , Fluorcarbonetos/análise , Caprilatos , Ácidos Alcanossulfônicos/análise
3.
Sci Total Environ ; 865: 161266, 2023 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-36592905

RESUMO

Perfluorooctanoic acid (PFOA) is widely used in industrial and consumer products of our daily life. It is well-documented that PFOA is closely associated with fatty liver disease. Recently, cumulating studies demonstrated the immunotoxicity of PFOA, but its harmful effect on the largest immune organ, spleen is still largely unknown. In the present study, we used PFOA-exposed mouse model together with comparative transcriptomic analysis to understand the molecular mechanisms underlying the immunotoxicity of PFOA. Furthermore, we investigated the possible use of vitamin C to reverse the PFOA-induced immunotoxicity in spleen. Our result showed that the PFOA exposure could reduce the spleen weight and plasma lymphocytes, and the splenic comparative transcriptomic analysis highlighted the alteration of cell proliferation, metabolism and immune response through the regulation of gene clusters including nicotinamide nucleotide transhydrogenases (NNT) and lymphocyte antigen 6 family member D and K (LY6D and LY6K). More importantly, the supplementation of vitamin C would relieve the PFOA-reduced spleen index and white blood cells. The bioinformatic analysis of transcriptome suggested its involvement in the spleen cell proliferation and immune response. For the first time, our study delineated the molecular mechanisms underlying the PFOA-induced immunotoxicity in the spleen. Furthermore, our results suggested that the supplementation of vitamin C had beneficial effect on the PFOA-altered spleen functions.


Assuntos
Fluorcarbonetos , Baço , Animais , Camundongos , Ácido Ascórbico/farmacologia , Caprilatos/toxicidade , Fluorcarbonetos/toxicidade
4.
J Hazard Mater ; 446: 130699, 2023 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-36603430

RESUMO

Perfluorinated-alkyl substances (PFAS) pose an unmet threat to the public because they are not strictly monitored and regulated. Perfluorinated-carbon alkyl chains (PFOA), a type of PFAS, at 70 fg/µL is the current health and safety recommendation. Current testing methods for PFOA and PFAS chemicals include HPLC-MS/MS and molecularly imprinted polymers, which are expensive, time-consuming, and require training. In this work, PFOA and PFOS detection was performed on a paper microfluidic chip using competitive interactions between PFOA/PFOS, cellulose fibers, and various reagents (L-lysine, casein, and albumin). Such interactions altered the surface tension at the wetting front and, subsequently, the capillary flow rate. A smartphone captured the videos of this capillary action. The samples flowed through the channel in less than 2 min. Albumin worked the best in detecting PFOA, followed by casein. The detection limit was 10 ag/µL in DI water and 1 fg/µL in effluent (processed) wastewater. Specificity to other non-fluorocarbon surfactants was also tested, using anionic sodium dodecyl sulfate (SDS), non-ionic Tween 20, and cationic cetrimonium bromide (CTAB). A combination of the reagents successfully distinguished PFOA from all three surfactants at 100% accuracy. This low-cost, handheld assay can be an accessible alternative for rapid in situ estimation of PFOA concentration.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Poluentes Químicos da Água , Poluentes Químicos da Água/análise , Espectrometria de Massas em Tandem , Ação Capilar , Smartphone , Caseínas , Tensoativos/análise , Fluorcarbonetos/análise , Ácidos Alcanossulfônicos/análise , Caprilatos/análise
5.
Chemosphere ; 315: 137653, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36581124

RESUMO

The global elimination and restriction of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS), respectively, have urged manufacturers to shift production to their substitutes which still pose threat to the environment with their bioaccumulation, toxicity and migration issues. In this context, efficient technologies and systematic mechanistic studies on the degradation of PFOA/PFOS substitutes are highly desirable. In this review, we summarize the progress in degrading PFOA/PFOS substitutes, including four kinds of mainstream methods. The pros and cons of the present technologies are analyzed, which renders the discussion of future prospects on rational optimizations. Additional discussion is made on the differences in the degradation of various kinds of substitutes, which is compared to the PFOA/PFOS and derives designing principles for more degradable F-containing compounds.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Caprilatos
6.
J Environ Sci (China) ; 127: 866-874, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36522114

RESUMO

Liquid-liquid extraction (LLE) using ionic liquids (ILs)-based methods to remove perfluoroalkyl chemicals (PFACs), such as perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS), from wastewater, is an important strategy. However, the lack of physicochemical and LLE data limits the selection of the most suitable ILs for the extraction of PFACs. In this work, 1763 ILs for PFACs extraction from water were systematically screened using COSMOtherm to estimate the infinite dilution activity coefficient (lnγ∞)of PFOA and PFOS in water and ILs. To evaluate the accuracy of COSMOtherm, 8 ILs with various lnγ∞ values were selected, and their extraction efficiency (E) and distribution coefficient (Dexp) were measured experimentally. The results showed that the predicted lnγ∞ decreased as the increase of experimental extraction efficiency of PFOA or PFOS, while the tendency of predicted distribution coefficient (Dpre) was consistent with the experimental (Dexp) results. This work provides an efficient basis for selecting ILs for the extraction of PFACs from wastewater.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Líquidos Iônicos , Caprilatos , Água
7.
Food Chem Toxicol ; 172: 113559, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36535450

RESUMO

PER: and polyfluoroalkyl substances (PFASs) have been associated with increased blood lipids in humans. Perfluorooctanoic acid (PFOA) has been also linked with elevated alanine transferase (ALT) serum levels in humans, and in rodents the liver is a main target organ for many PFASs. With the focus on New Approach Methodologies, the chronic oral equivalent effect doses were calculated for PFOA, PFNA (perfluorononanoic acid), PFHxS (perfluorohexanesulfonic acid) and PFOS (perfluorooctane sulfonic acid) based on in vitro effects measured in the HepaRG cell line. Selected in vitro readouts were considered biomarkers for lipid disturbances and hepatotoxicity. Concentration-response data obtained from HepaRG cells on triglyceride (TG) accumulation and expression changes of 12 selected genes (some involved in cholesterol homeostasis) were converted into corresponding human dose-response data, using physiologically based kinetic (PBK) model-facilitated reverse dosimetry. Next to this, the biokinetics of the chemicals were studied in the cell system. The current European dietary PFASs exposure overlaps with the calculated oral equivalent effect doses, indicating that the latter may lead to interference with hepatic gene expression and lipid metabolism. These findings illustrate an in vitro-in silico methodology, which can be applied for more PFASs, to select those that should be prioritized for further hazard characterization.


Assuntos
Ácidos Alcanossulfônicos , Poluentes Ambientais , Fluorcarbonetos , Humanos , Caprilatos/toxicidade , Lipídeos , Fluorcarbonetos/toxicidade
8.
Environ Res ; 219: 115024, 2023 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-36535390

RESUMO

Contaminated drinking water (DW) is a major source of exposure to per- and polyfluoroalkyl substances (PFAS) at locations around PFAS production/use facilities and military airports. This study aimed to investigate quantitative relationships between concentrations in DW and serum of nine perfluoroalkyl acids (PFAAs) in Swedish adult populations living near contamination hotspots. Short-chained (PFPeA, PFHxA, PFHpA, and PFBS) and long-chained PFAAs (PFOA, PFNA, PFDA, PFHxS and PFOS) were measured in DW and serum. We matched DW and serum concentrations for a total of 398 subjects living or working in areas receiving contaminated DW and in one non-contaminated area. Thereafter, linear regression analysis with and without adjustments for co-variates was conducted. This enabled to derive (i) serum concentrations at background exposure (CB) from sources other than local DW exposure (i.e. food, dust and textiles) at 0 ng/L DW concentration, (ii) population-mean PFAA serum:water ratios (SWR) and (iii) PFAA concentrations in DW causing observable elevated serum PFAA concentrations above background variability. Median concentrations of the sum of nine PFAAs ranged between 2.8 and 1790 ng/L in DW and between 7.6 and 96.9 ng/mL in serum. DW concentration was the strongest predictor, resulting in similar unadjusted and adjusted regression coefficients. Mean CB ranged from <0.1 (PFPeA, PFHpA, PFBS) to 5.1 ng/mL (PFOS). Serum concentrations increased significantly with increasing DW concentrations for all PFAAs except for PFPeA with SWRs ranging from <10 (PFHxA, PFHpA and PFBS) to 111 (PFHxS). Observed elevated serum concentrations above background variability were reached at DW concentrations between 24 (PFOA) and 357 ng/L (PFHxA). The unadjusted linear regression predictions agreed well with serum concentrations previously reported in various populations exposed to low and high DW levels of PFOA, PFHxS and PFOS. The quantitative relationships derived herein should be helpful to translate PFAA concentrations in DW to concentrations in serum at the population level.


Assuntos
Ácidos Alcanossulfônicos , Água Potável , Fluorcarbonetos , Poluentes Químicos da Água , Humanos , Adulto , Água Potável/análise , Suécia , Ácidos Alcanossulfônicos/análise , Caprilatos , Poluentes Químicos da Água/análise
9.
Chemosphere ; 313: 137622, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36565765

RESUMO

Perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) are widely detected in the environment and wild animals, thus posing a threat to wildlife and public health; however, knowledge about their immunotoxicity and the underlying mechanism remains limited. In the present study, male black-spotted frogs (Rana nigromaculata) were exposed to environmentally relevant concentrations (0, 1, and 10 µg/L) of PFOA or PFOS for 21 days; subsequently, biochemical analysis, molecular docking, and gene expression determination were conducted. The results indicated that exposure to 10 µg/L PFOA decreased the serum levels of immunoglobulin A. PFOS exposure significantly increased the hepatic levels of interleukin-1ß, interleukin-6, tumor necrosis factor-α, interferon-γ, and nitric oxide; but PFOA significantly increased the levels of only tumor necrosis factor-α. Furthermore, PFOA and PFOS exposure significantly decreased the activity of inducible nitric oxide synthase and total nitric oxide synthase. IBRv2 analysis indicated that PFOA and PFOS had a similar effect on these immune indicators, but PFOS was more toxic than PFOA. Molecular docking revealed that PFOA and PFOS can bind to nuclear factor-κB (NF-κB) by forming stable hydrogen bonds. PFOA and PFOS exposure upregulated the gene expression of NF-κB and its downstream genes. Significant correlations between the expression of genes involved in the NF-κB pathway and immune-related indicators suggests that PFOA- and PFOS-induced immunotoxicity was associated with the activation of NF-κB. Our findings provide novel insights into the potential role of NF-κB in immunotoxicity induced by PFOA and PFOS in frogs.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Animais , Masculino , NF-kappa B/genética , Fator de Necrose Tumoral alfa/genética , Simulação de Acoplamento Molecular , Ranidae/genética , Fluorcarbonetos/toxicidade , Caprilatos/toxicidade , Ácidos Alcanossulfônicos/toxicidade
10.
Chem Res Toxicol ; 35(12): 2252-2259, 2022 12 19.
Artigo em Inglês | MEDLINE | ID: mdl-36484463

RESUMO

Perfluorooctanoic acid is a manufactured material extensively utilized in industrial and consumer products. As a persistent organic pollutant, perfluorooctanoic acid has raised increasing public health concerns recently. Although perfluorooctanoic acid is known to induce lipid accumulation in the liver, the impact of perfluorooctanoic acid on different lipid classes has not been fully evaluated. In this study, we performed untargeted lipidomics analysis to investigate the impact of perfluorooctanoic acid on the lipid homeostasis in C57BL/6 male mice. Perfluorooctanoic acid disturbed the lipid profiles in serum and liver, with a variety of lipid classes significantly altered. Greater impacts were observed in the liver lipidome than the serum lipidome. In particular, some lipid clusters in the liver were altered by both high- and low-dose perfluorooctanoic acid exposure, including the increase of unsaturated triglycerides and the decrease of sphingomyelins, saturated phosphatidylcholines, saturated lysophosphatidylcholines, and phospholipid ethers. In parallel with an increase in the liver, a decrease of saturated phosphatidylcholines was found in the serum of high-dose perfluorooctanoic acid-treated mice. The findings from this study are helpful to improve the understanding of perfluorooctanoic acid-induced dysregulation of lipid metabolism and perfluorooctanoic acid-associated health effects in liver.


Assuntos
Caprilatos , Lipidômica , Masculino , Camundongos , Animais , Camundongos Endogâmicos C57BL , Caprilatos/toxicidade , Fígado/metabolismo , Metabolismo dos Lipídeos , Fosfatidilcolinas/metabolismo , Fosfatidilcolinas/farmacologia
11.
Int J Mol Sci ; 23(24)2022 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-36555799

RESUMO

The human body's natural protective barrier, the skin, is exposed daily to minor or major mechanical trauma, which can compromise its integrity. Therefore, the search for new dressing materials that can offer new functionalisation is fully justified. In this work, the development of two new types of dressings based on poly(3-hydroxyoctanoate) (P(3HO)) is presented. One of the groups was supplemented with conjugates of an anti-inflammatory substance (diclofenac) that was covalently linked to oligomers of hydroxycarboxylic acids (Oli-dicP(3HO)). The novel dressings were prepared using the solvent casting/particulate leaching technique. To our knowledge, this is the first paper in which P(3HO)-based dressings were used in mice wound treatment. The results of our research confirm that dressings based on P(3HO) are safe, do not induce an inflammatory response, reduce the expression of pro-inflammatory cytokines, provide adequate wound moisture, support angiogenesis, and, thanks to their hydrophobic characteristics, provide an ideal protective barrier. Newly designed dressings containing Oli-dicP(3HO) can promote tissue regeneration by partially reducing the inflammation at the injury site. To conclude, the presented materials might be potential candidates as excellent dressings for wound treatment.


Assuntos
Implantes Absorvíveis , Cicatrização , Camundongos , Humanos , Animais , Bandagens , Caprilatos
12.
Nutrients ; 14(24)2022 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-36558514

RESUMO

Introduction: Medium-chain fatty acids contain 6-12 carbon atoms and are absorbed directly into the blood vessels, proceeding to the portal vein and, finally, to the liver, where they are immediately utilized for energy. We aimed to determine the medium-chain fatty acid levels in women with and without breast cancer. Materials and Methods: A total of 200 women (100 breast cancer subjects and 100 control subjects) were recruited for the study as per the inclusion and exclusion criteria. Blood samples were collected for biochemical estimations. Fatty acid methyl esters were isolated, and medium-chain fatty acid levels in plasma were analyzed using gas chromatography (GC-FID). Statistical analysis was performed using SPSS 20.0 software; p ≤ 0.05 was considered statistically significant. Results: The fatty acid analysis revealed a significant decrease in the levels of caprylic acid (C:8) and lauric acid (C:12) and a significant increase in the level of capric acid (C:10) in the breast cancer subjects when compared to the control group. The level of caproic acid (C:6) was not significantly increased in the breast cancer subjects. In particular, the HER2- and ER-positive breast cancer subjects showed a decrease in their caprylic acid and lauric acid levels compared to other receptors. Conclusions: The results of the current study imply that lower levels of caprylic and lauric acid may be associated with a higher risk of breast cancer. The relevance of medium-chain fatty acids for preventive and therapeutic interventions will be amplified by further research on the possibility that alteration in a patient's medium-chain fatty acid composition may mechanistically contribute to disease progression or breast cancer risk.


Assuntos
Neoplasias da Mama , Caprilatos , Humanos , Feminino , Ácidos Graxos/análise , Ácidos Láuricos
14.
Ecotoxicol Environ Saf ; 248: 114314, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36436258

RESUMO

Per- and polyfluoroalkyl substances (PFAS) comprise a diverse class of chemicals used in industrial processes, consumer products, and fire-fighting foams which have become environmental pollutants of concern due to their persistence, ubiquity, and associations with adverse human health outcomes, including in pregnant persons and their offspring. Multiple PFAS are associated with adverse liver outcomes in adult humans and toxicological models, but effects on the developing liver are not fully described. Here we performed transcriptomic analyses in the mouse to investigate the molecular mechanisms of hepatic toxicity in the dam and its fetus after exposure to two different PFAS, perfluorooctanoic acid (PFOA) and its replacement, hexafluoropropylene oxide-dimer acid (HFPO-DA, known as GenX). Pregnant CD-1 mice were exposed via oral gavage from embryonic day (E) 1.5-17.5 to PFOA (0, 1, or 5 mg/kg-d) or GenX (0, 2, or 10 mg/kg-d). Maternal and fetal liver RNA was isolated (N = 5 per dose/group) and the transcriptome analyzed by Affymetrix Array. Differentially expressed genes (DEG) and differentially enriched pathways (DEP) were obtained. DEG patterns were similar in maternal liver for 5 mg/kg PFOA, 2 mg/kg GenX, and 10 mg/kg GenX (R2: 0.46-0.66). DEG patterns were similar across all 4 dose groups in fetal liver (R2: 0.59-0.81). There were more DEGs in fetal liver compared to maternal liver at the low doses for both PFOA (fetal = 69, maternal = 8) and GenX (fetal = 154, maternal = 93). Upregulated DEPs identified across all groups included Fatty Acid Metabolism, Peroxisome, Oxidative Phosphorylation, Adipogenesis, and Bile Acid Metabolism. Transcriptome-phenotype correlation analyses demonstrated > 1000 maternal liver DEGs were significantly correlated with maternal relative liver weight (R2 >0.92). These findings show shared biological pathways of liver toxicity for PFOA and GenX in maternal and fetal livers in CD-1 mice. The limited overlap in specific DEGs between the dam and fetus suggests the developing liver responds differently than the adult liver to these chemical stressors. This work helps define mechanisms of hepatic toxicity of two structurally unique PFAS and may help predict latent consequences of developmental exposure.


Assuntos
Fluorcarbonetos , Adulto , Humanos , Feminino , Gravidez , Camundongos , Animais , Fluorcarbonetos/toxicidade , Óxidos , Caprilatos/toxicidade , Feto , Polímeros
15.
Environ Health ; 21(1): 101, 2022 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-36289510

RESUMO

BACKGROUND: The endocrine disruption of perfluorinated compounds is an emerging issue. We aimed to examine the association of serum perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) levels with incident diabetes and fasting serum glucose concentration. METHODS: This prospective cohort study was based on an urban-based cohort subpopulation from the Korean Genome and Epidemiology Study. Serum samples (600 µL) were received from 100 participants in the normoglycemic baseline survey (2004-2013), and concentrations of PFOA and PFOS were measured using mass spectrometry. The incidence of diabetes was tracked in the follow-up survey (2012-2016). RESULTS: The mean age was 56.4 years (men, 59%). The median serum PFOA and PFOS concentrations were 4.29 ng/mL and 9.44 ng/mL, respectively. PFOA and PFOS concentrations differed according to age, sex, and residential area. After 60 months, 23 patients had diabetes. Log-transformed PFOA (lnPFOA) and log-transformed PFOS (lnPFOS) were significantly higher in those who transitioned to diabetes than in those who did not (both p < 0.05). After multivariate adjustment, lnPFOA (coefficient = 6.98, 95% CI -0.04-14, p = 0.054) and lnPFOS (coefficient = 7.06, 95% CI -0.96-15.08, p = 0.088) predicted increased fasting glucose without statistical significance. In addition, lnPFOA, but not lnPFOS, significantly predicted incident diabetes (HR = 3.98, 95% CI 1.42-11.1, p < 0.01). CONCLUSION: Exposure to PFOA and PFOS may have a potential dysglycemic effect. In particular, exposure to PFOA increased the risk of diabetes. Further research with larger sample size is warranted.


Assuntos
Ácidos Alcanossulfônicos , Diabetes Mellitus , Fluorcarbonetos , Adulto , Masculino , Humanos , Pessoa de Meia-Idade , Glucose , Jejum , Estudos Prospectivos , Caprilatos , Diabetes Mellitus/induzido quimicamente , Diabetes Mellitus/epidemiologia , Estudos de Coortes
16.
J Control Release ; 352: 163-178, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36314534

RESUMO

Drug delivery systems (DDS) for oral delivery of peptide drugs contain excipients that facilitate and enhance absorption. However, little knowledge exists on how DDS excipients such as permeation enhancers interact with the gastrointestinal mucus barrier. This study aimed to investigate interactions of the permeation enhancer sodium 8-[(2-hydroxybenzoyl)amino]octanoate (SNAC) with ex vivo porcine intestinal mucus (PIM), ex vivo porcine gastric mucus (PGM), as well as with in vitro biosimilar mucus (BM) by profiling their physical and barrier properties upon exposure to SNAC. Bulk mucus permeability studies using the peptides cyclosporine A and vancomycin, ovalbumin as a model protein, as well as fluorescein-isothiocyanate dextrans (FDs) of different molecular weights and different surface charges were conducted in parallel to mucus retention force studies using a texture analyzer, rheological studies, cryo-scanning electron microscopy (cryo-SEM), and single particle tracking of fluorescence-labelled nanoparticles to investigate the effects of the SNAC-mucus interaction. The exposure of SNAC to PIM increased the mucus retention force, storage modulus, viscosity, increased nanoparticle confinement within PIM as well as decreased the permeation of cyclosporine A and ovalbumin through PIM. Surprisingly, the viscosity of PGM and the permeation of cyclosporine A and ovalbumin through PGM was unaffected by the presence of SNAC, thus the effect of SNAC depended on the regional site that mucus was collected from. In the absence of SNAC, the permeation of different molecular weight and differently charged FDs through PIM was comparable to that through BM. However, while bulk permeation of neither of the FDs through PIM was affected by SNAC, the presence of SNAC decreased the permeation of FD4 and increased the permeation of FD150 kDa through BM. Additionally, and in contrast to observations in PIM, nanoparticle confinement within BM remained unaffected by the presence of SNAC. In conclusion, the present study showed that SNAC altered the physical and barrier properties of PIM, but not of PGM. The effects of SNAC in PIM were not observed in the BM in vitro model. Altogether, the study highlights the need for further understanding how permeation enhancers influence the mucus barrier and illustrates that the selected mucus model for such studies should be chosen with care.


Assuntos
Excipientes , Absorção Intestinal , Suínos , Animais , Excipientes/farmacologia , Caprilatos/análise , Caprilatos/metabolismo , Caprilatos/farmacologia , Ovalbumina/metabolismo , Sódio/metabolismo , Ciclosporina/farmacologia , Permeabilidade , Preparações Farmacêuticas/metabolismo , Muco/metabolismo , Peptídeos/metabolismo
17.
Environ Sci Technol ; 56(22): 15207-15219, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36314557

RESUMO

Many environmentally relevant poly-/perfluoroalkyl substances (PFASs) including perfluorooctane sulfonic acid (PFOS) and perfluorooctanoic acid (PFOA) exist in different isomeric (branched and linear) forms in the natural environment. The isomeric distribution of PFASs in the environment and source waters is largely controlled by the source of contamination and varying physicochemical properties imparted by their structural differences. For example, branched isomers of PFOS are relatively more reactive and less sorptive compared to the linear analogue. As a result, the removal of branched and linear PFASs during water treatment can vary, and thus the isomeric distribution in source waters can influence the overall efficiency of the treatment process. In this paper, we highlight the need to consider the isomeric distribution of PFASs in contaminated matrices while designing appropriate remediation strategies. We additionally summarize the known occurrence and variation in the physicochemical properties of PFAS isomers influencing their detection, fate, toxicokinetics, and treatment efficiency.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Purificação da Água , Fluorcarbonetos/química , Caprilatos/química , Isomerismo
18.
Environ Sci Technol ; 56(22): 15489-15498, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36279175

RESUMO

The transport of per- and polyfluoroalkyl substances (PFAS) in soil and groundwater is important for site investigation, risk characterization, and remediation planning. The adsorption of PFAS at air-water interfaces has been shown to significantly contribute to PFAS retention, with subsequent effects on concentrations and the time scales of transport. In this study, column experiments were conducted to investigate the transport of perfluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA), and 6:2 fluorotelomer sulfonate (6:2 FTS) individually and in binary mixtures in the presence of a trapped gas phase, using clean sands to isolate adsorption to air-water interfaces. Consistent with previous studies, the transport of PFOS, PFOA, and 6:2 FTS was retarded by adsorption at the air-water interface, with greater retention of PFOS due to its higher affinity for the air-water interface. Chromatographic separation occurred in the experiments using binary mixtures of PFOS and PFOA, with greater retention at lower influent concentrations. The mixture experiments also showed enhanced breakthrough of PFOA in the presence of PFOS, where effluent concentrations of PFOA were temporarily greater than the influent concentration prior to the breakthrough of PFOS. This enhanced breakthrough was attributed to competition between PFOS and PFOA for adsorption to the air-water interface.


Assuntos
Ácidos Alcanossulfônicos , Fluorcarbonetos , Porosidade , Caprilatos , Água
19.
Water Res ; 226: 119273, 2022 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-36283234

RESUMO

Perfluorooctanoic acid (PFOA), a "forever chemical", is continuously discharged and mitigated in the environment despite its production and use being severely restricted globally. Due to the transformation, attachment, and adsorption of PFOA in aquatic environments, PFOA accumulates in the porous media of sediments, soils, and vadose regions. However, the impact of trace PFOA in the porous media on interstitial water and water safety is not clear. In this work, we simulated a porous media layer using a sand column and explored the effects of µg-level PFOA migration on microbial community alternation, microbial function regulation, and the generation and spread of microbial risks. After 60 days of PFOA stimulation, Proteobacteria became the dominant phylum with an abundance of 91.8%, since it carried 71% of the antibiotic resistance genes (ARGs). Meanwhile, the halogen-related Dechloromonas abundance increased from 0.4% to 10.6%. In addition, PFOA significantly stimulated protein (more than 1288%) and polysaccharides (more than 4417%) production by up-regulating amino acid metabolism (p< 0.001) and membrane transport (p < 0.001) to accelerate the microbial aggregation. More importantly, the rapidly forming biofilm immobilized and blocked PFOA. The more active antioxidant system repaired the damaged cell membrane by significantly up-regulating glycerophospholipid metabolism and peptidoglycan biosynthesis. It is worth noting that PFOA increased the abundance of antibiotic resistance genes (ARGs) and human bacterial pathogens (HBPs) in porous media by 30% and 106%. PFOA increased the proportion of vertical transmission ARGs (vARGs), and co-occurrence network analysis (r ≥ 0.8, p ≤ 0.01) verified that vARGs were mainly mediated by HBPs. A comprehensive understanding of PFOA interactions with its microecological environment is provided.


Assuntos
Fluorcarbonetos , Microbiota , Humanos , Caprilatos , Bactérias/genética , Antibacterianos/farmacologia , Água , Genes Bacterianos
20.
Int J Mol Sci ; 23(19)2022 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-36233331

RESUMO

Glycolipids can be synthetized in deep eutectic solvents (DESs) as they possess low water content allowing a reversed lipase activity and thus enables ester formation. Based on this principle, honey can also serve as a media for glycolipid synthesis. Indeed, this supersaturated sugar solution is comparable in terms of physicochemical properties to the sugar-based DESs. Honey-based products being commercially available for therapeutic applications, it appears interesting to enhance its bioactivity. In the current work, we investigate if enriching medical grade honey with in situ enzymatically-synthetized glycolipids can improve the antimicrobial property of the mixture. The tested mixtures are composed of Manuka honey that is enriched with octanoate, decanoate, laurate, and myristate sugar esters, respectively dubbed GOH, GDH, GLH, and GMH. To characterize the bioactivity of those mixtures, first a qualitative screening using an agar well diffusion assay has been performed with methicillin-resistant Staphylococcus aureus, Bacillus subtilis, Candida bombicola, Escherichia coli, and Pseudomonas putida which confirmed considerably enhanced susceptibility of these micro-organisms to the different glycolipid enriched honey mixtures. Then, a designed biosensor E. coli strain that displays a stress reporter system consisting of three stress-specific inducible, red, green, and blue fluorescent proteins which respectively translate to physiological stress, genotoxicity, and cytotoxicity was used. Bioactivity was, therefore, characterized, and a six-fold enhancement of the physiological stress that was caused by GOH compared to regular Manuka honey at a 1.6% (v/v) concentration was observed. An antibacterial agar well diffusion assay with E. coli was performed as well and demonstrated an improved inhibitory potential with GOH upon 20% (v/v) concentration.


Assuntos
Anti-Infecciosos , Mel , Staphylococcus aureus Resistente à Meticilina , Ágar , Antibacterianos/análise , Antibacterianos/farmacologia , Anti-Infecciosos/farmacologia , Caprilatos , Decanoatos , Escherichia coli , Ésteres , Glicolipídeos/farmacologia , Lauratos , Lipase , Testes de Sensibilidade Microbiana , Miristatos , Açúcares , Água
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