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1.
Int J Hyg Environ Health ; 257: 114346, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38447259

RESUMO

BACKGROUND: Studies on cognitive and neurodevelopmental outcomes have shown inconsistent results regarding the association with prenatal exposure to perfluoroalkyl substance (PFAS) and organochlorines. Assessment of mixture effects of correlated chemical exposures that persist in later life may contribute to the unbiased evaluation and understanding of dose-response associations in real-life exposures. METHODS: For a subset of the 4th Flemish Environment and Health Study (FLEHS), concentrations of four PFAS and six organochlorines were measured in respectively 99 and 153-160 cord plasma samples and 15 years later in adolescents' peripheral serum by Ultra Performance Liquid Chromatography-Tandem Mass Spectrometry (UPLC-MS/MS). Sustained and selective attention were measured at 14-15 years with the Continuous Performance Test (CPT) and Stroop Test as indicators of potential neurodevelopmental deficits. Quantile g-computation was applied to assess the joint associations between prenatal exposure to separate and combined groups of PFAS and organochlorines and performance in the CPT and Stroop Test at adolescence. Subsequently, individual effects of each chemical compound were analyzed in mixed effects models with two sets of covariates. Analytical data at birth and at the time of cognitive assessment allowed for off-setting postnatal exposure. RESULTS: In mixtures analysis, a simultaneous one-quantile increase in the natural log-transformed values of PFAS and organochlorines combined was associated with a decrease in the mean reaction time (RT) and the reaction time variability (RTV) in the CPT (ß = -15.54, 95% CI:-29.64, -1.45, and ß = -7.82, 95% CI: -14.97, -0.67 respectively) and for the mixture of PFAS alone with RT (ß = -11.94, 95% CI: -23.29, -0.60). In the single pollutant models, these results were confirmed for the association between perfluorohexanesulfonate (PFHxS) with RT (ß = -17.95, 95% CI = -33.35, -2.69) and hexachlorobenzene with RTV in the CPT (ß = -5.78, 95% CI: -10.39, -0.76). Furthermore, the participants with prenatal exposure above the limit of quantification for perfluorononanoic acid (PFNA) had a significantly shorter RT and RTV in the CPT (ß = -23.38, 95% CI: -41.55, -5.94, and ß = -9.54, 95% CI: -19.75, -0.43, respectively). CONCLUSION: Higher prenatal exposure to a PFAS mixture and a mixture of PFAS and organochlorines combined was associated with better sustained and selective attention during adolescence. The associations seemed to be driven by PFHxS and were not linked to exposure levels at the time of assessment.


Assuntos
Ácidos Alcanossulfônicos , Poluentes Ambientais , Fluorocarbonos , Efeitos Tardios da Exposição Pré-Natal , Feminino , Gravidez , Recém-Nascido , Humanos , Adolescente , Cromatografia Líquida , Espectrometria de Massas em Tandem , Cognição
2.
Toxicol Sci ; 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38419586

RESUMO

There is growing evidence indicating the substantial contribution of man-made products to an increase in the risk of diseases of civilization. In this article, the Belgian Scientific Registration, Evaluation, Authorization and restriction of CHemicals (REACH) Committee gives a critical view on the working of REACH. The current regulatory framework needs to further evolve taking into account data generated using modern science and technology. There is a need for improved assessment process not only before but also after entering the market. Objectivity, transparency, and the follow-up after market access can be optimized. Additionally, no guidance documents exist for regulation of mixture effects. Further, the lengthiness before regulatory action is a big concern. Decision making often takes several years leading to uncertainties for both producers and end users. A first proposed improvement is the implementation of independent toxicity testing, to assure objectivity, transparency, and check and improve compliance. A "no data, no market" principle could prevent access of hazardous chemicals to the market. Additionally, the introduction of novel testing could improve information on endpoints such as endocrine disrupting abilities, neurotoxicity, and immunotoxicity. An adapted regulatory framework that integrates data from different sources and comparing the outputs with estimates of exposure is required. Fast toxicology battery testing and toxicokinetic testing could improve speed of decision making. Hereby, several improvements have been proposed that could improve the current REACH legislation.

3.
J Hazard Mater ; 466: 133547, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38262324

RESUMO

Identification of key As mobilization processes in estuarine sediments is challenging due to the transitional hydrodynamic condition and the technical restriction of obtaining fine-scale results. Herein, high-resolution (µm to mm) and in situ profiling of As with associated elements (Fe, Mn, and S) by the diffusive gradients in thin-film (DGT) technique were applied and coupled with pore water and solid phase analysis as well as microbial high-throughput sequencing, to ascertain the driving mechanisms of As mobilization in the sediments of Pearl River Estuary (PRE). Significant diffusion fluxes of As from sediment to water were observed, particularly in the upper estuary. With the seaward increase of salinity, the driving mechanism of As mobilization gradually shifted from microbial-induced dissimilatory Fe reduction to saltwater-induced ion exchange. Correspondingly, the dominant Fe-reducing bacteria (FeRB) in sediments changed from the genera Clostridium_sensu_stricto_1 and Bacillus to Ferrimonas and Deferribacter. The presence of dissolved sulfide in deeper sediments contributes to As removal through the formation of As-S precipitates as supported by theoretical calculations. Fine-scale findings revealed seaward changes of As mobilization mechanism in the sediments of a human-impacted estuary and may benefit the understanding of As biogeochemical behavior in estuaries worldwide.

4.
J Hazard Mater ; 465: 133209, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38101023

RESUMO

In this study, the vertical distribution of mercury (Hg) in estuarine and marine sediment porewaters and solid phases was assessed by conventional and passive sampling techniques in the historically polluted Scheldt Estuary and Belgian Coastal Zone (BCZ). The Diffusive Gradients in Thin-films (DGT) measured labile Hg concentrations (HgLA) were mostly lower than the porewater Hg concentrations (HgPW), and they also presented different vertical distribution patterns. Still high Hg concentrations in the sediment solid phases, comparable to the historical ones, were observed. Even though pH, redox potential and dissolved sulfide concentration could influence the Hg biogeochemical behaviour, organic matter (OM) played a key role in governing Hg mobilization from sediment solid phase to porewater and in its partitioning between porewater and solid phase over depth. In the marine sediments, where OM had a marine signature, higher labile Hg concentrations in the porewater and faster resupply from the solid phase were observed. The DGT technique showed significant potential not only for the measurement of bioavailable Hg fractions in porewater, but also for the assessment of kinetic parameters governing the release of labile Hg species from the solid phase with the assistance of the DGT Induced Fluxes in Sediments (DIFS) model.

5.
Environ Sci Technol ; 57(20): 7840-7848, 2023 05 23.
Artigo em Inglês | MEDLINE | ID: mdl-37183959

RESUMO

Determining species, concentrations, and physicochemical parameters in natural waters is key to improve our understanding of the functioning of these ecosystems. Diffusive Gradients in Thin-films (DGT) devices with different thicknesses of the resin or of the diffusive disc can be used to collect independent information on relevant parameters. In particular, DGT devices with a stack of two resin discs offer a simple way to determine dissociation rate constants of metal complexes from the accumulation of the target metal in the back resin disc. In this work, simple approximate expressions for the determination of the dissociation rate constant are reported and applied to a model Ni nitrilotriacetic complex as well as to Zn complexes in the Mediterranean Osor stream. Once the physicochemical parameters are known, one can plot the labile fraction of the metal complexes in terms of the thickness of the diffusion domain. These plots reveal a strong dependence on the nature of complexes as well as on the characteristics of the diffusion domain, and they are of high interest as predictors of availability to biota whose uptake is limited by diffusion.


Assuntos
Complexos de Coordenação , Ecossistema , Metais/análise , Difusão , Biota , Monitoramento Ambiental
6.
Sci Total Environ ; 882: 163604, 2023 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-37087008

RESUMO

The geochemical behavior of metals in water and sediment was investigated in the tidal section of the Zenne River in Belgium. Twelve-hour sampling campaigns were performed in October 2013 and March 2021 at the mouth of the Zenne River, under dry and rainy weather conditions respectively. Water samples were collected every hour while the passive samplers of Diffusive Gradients in Thin-films (DGT) were deployed continuously during a tidal cycle. In addition, bottom sediments were sampled at the tidal station and water samples were taken upstream and downstream of that station to identify the metal sources. The highest concentrations of Fe, Mn, Pb, Cr, Ni and Zn appear at low tide, indicating the Zenner River as a main source. However, for Co, Cd and Cu, other sources including upstream transport may explain their behavior during a tidal cycle. Fe, Pb and Cr are essentially transported in the particulate phase (<10 % dissolved) while the other metals in the dissolved phase (20 to 90 %). Rainfall and wind gust events also play an important role in trace metal distribution, increasing sediment resuspension and metal desorption. A good agreement was found between the time-averaged dissolved and DGT-labile metal concentrations with the exception of Cu and Fe, which form strong organic Cu complexes and Fe colloids respectively. The sediments of the tidal Zenne are contaminated by trace metals, thus acting as a secondary pollution source to the river. The reductive dissolution of Mn and Fe oxyhydroxides and the release of associated trace metals are the main mobilization mechanisms. Knowledge of the upstream and downstream levels in the water column, the benthic fluxes, which are based on turbulent diffusion, and the partitioning between dissolved and particulate phases allow to explain the metal concentration variations during the tidal cycle.

7.
Sci Total Environ ; 878: 163019, 2023 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-36996990

RESUMO

Estuaries and coastal zones are areas with complex biogeochemical and hydrological cycles and are generally facing intense pollution due to anthropogenic activities. An emblematic example is the Scheldt Estuary which ends up in the North Sea and has been historically heavily contaminated by multiple pollutants, including mercury (Hg). We report here Hg species and their levels in surface waters of the Scheldt Estuary and the Belgian Part of North Sea (BPNS) from different sampling campaigns in February-April 2020 and 2021. Along the estuary, Hg concentration on suspended particles ([HgSPM]) progressively decreased with increasing salinity and was strongly correlated with organic matter content (%Corg) and origin (identified with δ13Corg). While [HgSPM] drives total Hg concentration in the estuary (total dissolved Hg, HgTD is only 7 ± 6 %), annual and daily variations of total Hg levels were mostly attributed to changes in SPM loads depending on river discharge and tidal regime. In the BPNS, a significant fraction of total Hg occurs as HgTD (40 ± 21 %) and the majority of this HgTD was reducible (i.e. labile Hg), meaning potentially available for microorganisms. Compared to the '90s, a significant decrease of [HgSPM] was observed in the estuary, but this was not the case for [HgTD], which can be due to (1) still significant discrete discharges from Antwerp industrial area, and (2) higher Hg partitioning towards the dissolved phase in the water column relative to the '90s. Our results highlight the important contribution of the Scheldt estuary for the Hg budget in North Sea coastal waters, as well as the need for seasonal monitoring of all Hg species.

8.
Int J Hyg Environ Health ; 248: 114115, 2023 03.
Artigo em Inglês | MEDLINE | ID: mdl-36689783

RESUMO

The European Joint Programme HBM4EU coordinated and advanced human biomonitoring (HBM) in Europe in order to provide science-based evidence for chemical policy development and improve chemical management. Arsenic (As) was selected as a priority substance under the HBM4EU initiative for which open, policy relevant questions like the status of exposure had to be answered. Internal exposure to inorganic arsenic (iAs), measured as Toxic Relevant Arsenic (TRA) (the sum of As(III), As(V), MMA, DMA) in urine samples of teenagers differed among the sampling sites (BEA (Spain) > Riksmaten adolescents (Sweden), ESTEBAN (France) > FLEHS IV (Belgium), SLO CRP (Slovenia)) with geometric means between 3.84 and 8.47 µg/L. The ratio TRA to TRA + arsenobetaine or the ratio TRA to total arsenic varied between 0.22 and 0.49. Main exposure determinants for TRA were the consumption of rice and seafood. When all studies were combined, Pearson correlation analysis showed significant associations between all considered As species. Higher concentrations of DMA, quantitatively a major constituent of TRA, were found with increasing arsenobetaine concentrations, a marker for organic As intake, e.g. through seafood, indicating that other sources of DMA than metabolism of inorganic As exist, e.g. direct intake of DMA or via the intake of arsenosugars or -lipids. Given the lower toxicity of DMA(V) versus iAs, estimating the amount of DMA not originating from iAs, or normalizing TRA for arsenobetaine intake could be useful for estimating iAs exposure and risk. Comparing urinary TRA concentrations with formerly derived biomonitoring equivalent (BE) for non-carcinogenic effects (6.4 µg/L) clearly shows that all 95th percentile exposure values in the different studies exceeded this BE. This together with the fact that cancer risk may not be excluded even at lower iAs levels, suggests a possible health concern for the general population of Europe.


Assuntos
Arsênio , Arsenicais , Adolescente , Humanos , Arsênio/análise , Arsenicais/urina , Europa (Continente) , França , Exposição Ambiental/análise
9.
Sci Total Environ ; 839: 156353, 2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-35654196

RESUMO

The biogeochemical cycle of trace metals and oxyanions in marine sediments is mainly controlled by early diagenesis of organic material, but anthropogenic activities such as dumping of dredged sludge or shipyard activities can strongly perturb these natural processes. Therefore, the impact of dumping of dredged sludge, shipyard activities such as blasting of boat hulls and the mixing of polluted Scheldt estuary water with less polluted coastal water on the mobilization of trace metals and oxyanions in the sediments was studied in the pre- and post-bloom period (March and October) in Belgian Coastal Zone (BCZ). Vertical profiles of total and labile dissolved trace element concentrations, dissolved sulfide, pH and redox potential were assessed in sediment porewaters. Generally, total and labile dissolved element profiles in the porewaters are well correlated, showing higher concentrations in March when the redox potential is lower and sulfide concentrations higher. Low pH levels were documented together with high amounts of Fe and associated elements in March at the dumping station. At the coastal station in the vicinity of the shipyards, sediment porewaters are enriched in dissolved Zn while at the mouth of the Scheldt estuary the highest dissolved Cu levels were found. Theoretical calculations with Visual MINTEQ confirm the increased Fe and associated element concentrations in March (lower pH) and the lower metal concentrations in October (lower Eh). R values, ratio of labile dissolved to total dissolved concentrations, reflect the potential of the solid sediment phase to supply labile elements to the porewater. They were lowest for Cu and highest for V. This study showed that anthropogenic activities in the BCZ such as dumping of dredged sludge and blasting of boat hulls have a serious impact on the levels, distribution and bioavailability of contaminants in the sediments, which may form a real threat to the benthic ecosystem.


Assuntos
Metais Pesados , Oligoelementos , Poluentes Químicos da Água , Efeitos Antropogênicos , Ecossistema , Monitoramento Ambiental , Sedimentos Geológicos , Metais Pesados/análise , Esgotos , Sulfetos , Oligoelementos/análise , Água , Poluentes Químicos da Água/análise
10.
Water Res ; 214: 118189, 2022 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-35184019

RESUMO

Effluents of sewage treatment plants (STPs) are an important source of estrogenic substances to the receiving water bodies affecting their ecological safety. In this study, steroids, bisphenol A (BPA) and phthalates were assessed in the secondary (SE) and tertiary effluent (TE) of three typical urban STPs in Beijing (China). In addition, the overall estrogenic activity in these effluents was assessed by an in-vitro bioassay (ERE-CALUX). Results showed that the concentrations and activities of estrogenic compounds in TE were lower than those in SE. The residual concentration of 17ß-estradiol (E2) was the highest among the detected steroids, accounting for 51.6 ± 5.1% in SE and 57.5 ± 24.8% in TE. The residual level (25.2-41.6 ng/L) of BPA in effluents was significantly higher than that of steroids (0.2-28.8 ng/L). The residual concentration of diethyl phthalate was the highest among the detected phthalates accounting for 47.1 ± 5.1% in SE and 37.6 ± 11.5% in TE. Steroids and BPA had a higher removal rate (83.5% and 96.7%) in secondary and tertiary treatment than phthalates (68.8% and 83.1%). The hydrophobic characteristics of these estrogenic compounds determined the removal mechanism. The removal of steroids, BPA, dimethyl phthalate and diethyl phthalate (LogKow= 1.61-4.15) mainly occurred through biodegradation in the water phase, while the removal of dibutyl phthalate, butylbenzyl phthalate and di(2-ethylhexyl) phthalate (LogKow= 4.27-7.50) mainly occurred in the solid phase after adsorption on and sedimentation of the suspended particulate matter. According to ERE-CALUX, the estrogenic activity in the final STP effluents was 3.2-45.6 ng E2-equivalents/L, which is higher than reported levels in the effluents of European STPs. Calculation of estrogenic equivalents by using substance specific chemical analysis indicated that the dominant contributor was E2 (56.4-88.4%), followed by 17α-ethinylestradiol (EE2) (4.1-34.8%), both also exerting a moderate risk to the aquatic ecosystem. While the upgrade of treatment processes in STPs has efficiently reduced the emission of estrogenic substances, their ecological risk was not yet phased out.

11.
Int J Hyg Environ Health ; 240: 113895, 2022 03.
Artigo em Inglês | MEDLINE | ID: mdl-34883335

RESUMO

BACKGROUND/AIM: Glyphosate, a broad-spectrum herbicide, and its main metabolite aminomethylphosphonic acid (AMPA) are persistent in the environment. Studies showed associations between glyphosate or AMPA exposure and several adverse cellular processes, including metabolic alterations and oxidative stress. OBJECTIVE: To determine the association between glyphosate and AMPA exposure and biomarkers of biological aging. METHODS: We examined glyphosate and AMPA exposure, mtDNA content and leukocyte telomere length in 181 adults, included in the third cycle of the Flemish Environment and Health Study (FLEHSIII). DNA was isolated from leukocytes and the relative mtDNA content and telomere length were determined using qPCR. Urinary glyphosate and AMPA concentrations were measured by Gas Chromatography-Tandem Mass Spectrometry (GC-MS-MS). We used multiple linear regression models to associate mtDNA content and leukocyte telomere length with glyphosate or AMPA exposure while adjusting for confounding variables. RESULTS: A doubling in urinary AMPA concentration was associated with 5.19% (95% CI: 0.49 to 10.11; p = 0.03) longer leukocyte telomere length, while no association was observed with urinary glyphosate concentration. No association between mtDNA content and urinary glyphosate nor AMPA levels was observed. CONCLUSIONS: This study showed that AMPA exposure may be associated with telomere biology in adults.


Assuntos
Herbicidas , Biomarcadores , Glicina/análogos & derivados , Herbicidas/urina , Organofosfonatos , Ácido alfa-Amino-3-hidroxi-5-metil-4-isoxazol Propiônico
12.
Artigo em Inglês | MEDLINE | ID: mdl-34067438

RESUMO

Human biomonitoring (HBM) monitors levels of environmental pollutants in human samples, which often is a topic of concern for residents near industrially contaminated sites (ICSs). Around an ICS area in Menen (Belgium), including a (former) municipal waste incinerator and a metal recovery plant, increasing environmental concentrations of dioxins and polychlorinated biphenyls (PCBs) were observed, causing growing concern among residents and authorities. The local community succeeded in convincing the responsible authorities to investigate the problem and offer research funding. Persistent organic pollutants (POPs) were measured in two consecutive HBM studies (2002-2006 and 2010-2011), in the context of the Flemish Environment and Health Study (FLEHS), as well as in soil and locally produced food. Meanwhile, local authorities discouraged consumption of locally produced food in a delineated area of higher exposure risk. Ultimately, HBM and environmental data enabled tailored dietary recommendations. This article demonstrates the usefulness of HBM in documenting the body burdens of residents near the ICS, identifying exposure routes, evaluating remediating actions and providing information for tailored policy strategies aiding to further exposure reduction. It also highlights the role of the local stakeholders as an example of community-based participatory research and how such an approach can create societal support for research and policy.


Assuntos
Dioxinas , Poluentes Ambientais , Bifenilos Policlorados , Bélgica , Monitoramento Biológico , Monitoramento Ambiental , Poluentes Ambientais/análise , Humanos , Políticas , Bifenilos Policlorados/análise
13.
Front Chem ; 9: 624511, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-33889563

RESUMO

The speciation of trace metals in an aquatic system involves the determination of free ions, complexes (labile and non-labile), colloids, and the total dissolved concentration. In this paper, we review the integrated assessment of free ions and labile metal complexes using Diffusive Gradients in Thin-films (DGT), a dynamic speciation technique. The device consists of a diffusive hydrogel layer made of polyacrylamide, backed by a layer of resin (usually Chelex-100) for all trace metals except for Hg. The best results for Hg speciation are obtained with agarose as hydrogel and a thiol-based resin. The diffusive domain controls the diffusion flux of the metal ions and complexes to the resin, which strongly binds all free ions. By using DGT devices with different thicknesses of the diffusive or resin gels and exploiting expressions derived from kinetic models, one can determine the labile concentrations, mobilities, and labilities of different species of an element in an aquatic system. This procedure has been applied to the determination of the organic pool of trace metals in freshwaters or to the characterization of organic and inorganic complexes in sea waters. The concentrations that are obtained represent time-weighted averages (TWA) over the deployment period.

14.
Chemosphere ; 272: 129891, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33601208

RESUMO

Soil management and cultivar selection are two strategies to reduce the accumulation risk of heavy metals in crops. However, it is still an open question which of these two strategies is more efficient for the safe utilization of contaminated soil. In this study, the available bio-concentration factors (aBCF) of arsenic (As) and cadmium (Cd) among 39 maize cultivars were determined through a field experiment. The effect of soil management was mimicked by choosing diverse sampling sites having different soil available contents of As and Cd. The aBCF of As and Cd in grain ranged from 0.02 to 0.13 and 1.17 to 42.2, respectively. The accumulation ability of As and Cd was classified among different maize cultivars. Soil pH and total As controlled the level of available As in soils, while soil pH dominated available Cd in soil. A soil pH of 6.5 was recommended to simultaneously minimize soil available As and Cd by managing soil conditions. The quantitative effects of cultivar and soil management on grain As and Cd were expressed as Q [Grain As] = 0.746Q [Cultivar]-0.126Q [pH]+0.276Q [Asavailable] (R2 = 0.648, P = 1.00 × 10-37) and Q [Grain Cd] = 0.913Q [Cultivar]-0.192Q [pH]+0.071Q [SOC] (R2 = 0.782, P = 1.00 × 10-37), respectively. Cultivar selection contributed stronger than soil management to decrease the As and Cd levels in maize grains. A feasible method to seek for a more efficient strategy was proposed for the safe utilization of contaminated soil.


Assuntos
Arsênio , Oryza , Poluentes do Solo , Cádmio/análise , Solo , Poluentes do Solo/análise , Zea mays
15.
Sci Total Environ ; 757: 143827, 2021 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-33257074

RESUMO

The biogeochemical behavior of Cd, Co, Cr, Cu, Ni and Pb along the historically polluted Scheldt estuary (Belgium - The Netherlands) was investigated in this study. As never studied before in this area, labile trace metals were measured using the passive sampling technique of Diffusive Gradients in Thin-films (DGT), while total dissolved and particulate trace metal concentrations were assessed using classic active sampling techniques. This dual approach allowed us to highlight the variations of trace metal speciation and distribution in the estuarine surface waters, considering environmental and physicochemical gradients along the transect. The large data set obtained was then compared with literature data of historical measurements along the Scheldt (from 1980 until now), but also from other estuaries. As emphasized by our results, trace metal mobility and partitioning along the Scheldt estuary was mainly driven by biogeochemical reactions which were strongly influenced by gradients of specific estuarine physico-chemical parameters, such as salinity, turbidity, temperature and so on. Hence, all species of trace metals displayed a non-conservative behavior. More precisely, dissolved labile fractions of trace metals showed higher levels in the middle estuary, where many solubilization and remobilization processes occurred due to turbulent mixing mechanisms and an increasing salinity. Our study confirmed the decreasing trend historically observed for particulate metals along the Scheldt, as well as the rising concentrations recorded for dissolved trace metals which might also lead to an increase of their labile fraction measured by the DGT. Finally, these preliminary results suggested that a more regular monitoring of labile metal along the Scheldt estuary is essential to have an in-depth understanding of trace metal speciation and to review bioavailability of trace metals within estuarine ecosystems.

16.
Environ Sci Technol ; 54(23): 15151-15161, 2020 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-33170658

RESUMO

Different mobilization mechanisms control the metal distribution in surface sediments of the Belgium coastal zone (BCZ) and the anoxic Gotland basin (GB). This mobilization was studied using DGT (diffusive gradients in thin films): vertical one-dimensional (1D) profiles of Cd, Co, Cu, Fe, Mn, Ni, Pb, and Zn were measured at 5 mm intervals, while two-dimensional (2D) high-resolution (100 µm) images of smaller zones of the sediment profile were obtained on separate DGT probes. Removal of dissolved Cd, Cu, and Pb in BCZ sediments caused steep vertical gradients at the sediment-water interface that were well replicated in 1D profiles and 2D images. While 1D profiles showed apparent coincident maxima of Co, Mn, and Fe, 2D images revealed mutually exclusive Co and Fe mobilization. Correlation analysis supported this observation and showed a consistent linkage between Co and Mn. Sharp maxima of some metals in the vertical 1D profiles of GB sediment were attributed to localized mobilization in microniches. Examination of an ∼1 mm diameter Cu and Ni maximum in 2D, defined by ∼300 data points, showed that the metals were supplied from localized decomposition of reactive organic material, rather than from reductively dissolving Fe or Mn oxides, and that they were removed as their sulfides.


Assuntos
Metais Pesados , Oligoelementos , Poluentes Químicos da Água , Bélgica , Monitoramento Ambiental , Sedimentos Geológicos , Metais Pesados/análise , Poluentes Químicos da Água/análise
17.
Environ Int ; 145: 106149, 2020 12.
Artigo em Inglês | MEDLINE | ID: mdl-33002701

RESUMO

BACKGROUND AND AIMS: Prenatal chemical exposure has frequently been associated with reduced fetal growth although results have been inconsistent. Most studies associate single pollutant exposure to this health outcome, even though this does not reflect real life situations as humans are exposed to many pollutants during their life time. The objective of this study is to investigate the association between prenatal exposure to a mixture of persistent environmental chemicals and birth weight using multipollutant models. METHODS: We combined exposure biomarker data measured in cord blood samples of 1579 women from four Flemish birth cohorts collected over a 10 years' time period. The common set of available and detectable exposure measures in these cohorts are three polychlorinated biphenyls (PCB) congeners (138, 153 and 180), hexachlorobenzene (HCB), dichlorodiphenyldichloroethylene (p,p'-DDE) and the metals cadmium and lead. Multiple linear regression (MLR), Bayesian Information Criterion (BIC), penalized regression using minimax concave penalty (MCP) and Bayesian Adaptive Sampling (BAS) were applied to assess the influence of multiple pollutants in a single analysis on birth weight, adjusted for a priori selected covariates. RESULTS: In the pooled dataset, a median (P25-P75) birth weight and gestational age of 3420 (3140-3700) grams and 39 (39-40) weeks was observed respectively. The median contaminant levels in cord blood were: 15.8, 26.5, 18.0, 16.9 and 91.5 ng/g lipid for PCB 138, PCB 153, PCB 180, HCB and p,p'-DDE, respectively, 0.075 µg/L for cadmium and 9.7 µg/L for lead. According to the applied statistical methods for multipollutant assessment, p,p'-DDE and PCB 180 were most consistently associated with birth weight. In addition, PCB 153 was selected when applying MCP and BAS. An inverse association with birth weight was found for the PCB congeners, while an increased birth weight was observed for elevated levels of p,p'-DDE. CONCLUSIONS: Assessing the health risk of combinations of exposure biomarkers reflects better real-world situations and thereby allows more effective risk assessment. Our results add to the existing evidence based on detrimental effects of PCBs on birth weight and indicate a possible increase in birth weight due to p,p'-DDE (while correcting for PCBs).


Assuntos
Poluentes Ambientais , Bifenilos Policlorados , Teorema de Bayes , Peso ao Nascer , Diclorodifenil Dicloroetileno/análise , Poluentes Ambientais/análise , Feminino , Humanos , Poluentes Orgânicos Persistentes , Bifenilos Policlorados/análise , Bifenilos Policlorados/toxicidade , Gravidez
18.
Environ Int ; 145: 106140, 2020 12.
Artigo em Inglês | MEDLINE | ID: mdl-32966951

RESUMO

Belgian coastal sediment serves as an important sink for trace elements, yet a systematic study covering a wide range of elements including redox-sensitive metals (Fe, Mn, and Co), cationic trace metals (Cd, Pb, Ni, Cu, and Zn), oxyanions (P, V, As, and Mo), and sulfide has not been performed and the mechanisms controlling their mobilization were not investigated. Here, a passive sampling technique, Diffusive Gradients in Thin-films (DGT), was used in situ to obtain high resolution concentration profiles of these elements in the sediment porewater. Our results revealed two mobilization mechanisms of cationic trace metals and oxyanions in Belgian coastal sediments, both strongly linked to the cycling of Fe. Mobilization of Co, Pb, Ni, and Cu is controlled by electrogenic sulfur oxidation, acidification of the porewater and dissolution of FeS, while that of oxyanions (P, V, and As) is controlled by reductive dissolution of Fe oxyhydroxides. Constant cationic trace metal to Fe molar ratios were established in FeS, while the oxyanion to Fe ratios in Fe oxyhydroxides differ significantly between sampling stations, which is primarily caused by competing effects. We found no evidence that cationic trace metal mobilization was related to Fe oxyhydroxides, or oxyanion mobilization to FeS. This suggests that particulate organic matter forms the major pathway for cationic trace metal input in coastal sediments and that oxyanions will not be incorporated in FeS but form their own oxyanion-sulfide compound. These findings will contribute to a better understanding of the mobilization mechanisms of cationic trace metals and oxyanions in coastal sediments, and of their biogeochemical cycling in coastal ecosystems.


Assuntos
Metais Pesados , Poluentes Químicos da Água , Bélgica , Ecossistema , Monitoramento Ambiental , Sedimentos Geológicos , Metais Pesados/análise , Poluentes Químicos da Água/análise
19.
Sci Rep ; 10(1): 387, 2020 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-31941967

RESUMO

Nutrition during early childhood is linked to metabolic programming. We hypothesized that breastfeeding has long-term consequences on the energy metabolism exemplified by mitochondrial DNA (mtDNA). As part of the third cycle of the Flemish Environment and Health Study (FLEHSIII) cohort, 303 adolescents aged 14-15 years were included. We associated breastfeeding and blood mtDNA content 14-15 years later while adjusting for confounding variables. Compared with non-breastfed adolescents, mtDNA content was 23.1% (95%CI: 4.4-45.2; p = 0.013) higher in breastfed adolescents. Being breastfed for 1-10 weeks, 11-20 weeks, and >20 weeks, was associated with a higher mtDNA content of respectively 16.0% (95%CI: -7.1-44.9; p = 0.191), 23.5% (95%CI: 0.8-51.3; p = 0.042), and 31.5% (95%CI: 4.3-65.7; p = 0.021). Our study showed a positive association between breastfeeding and mtDNA content in adolescents which gradually increased with longer periods of breastfeeding. Higher mtDNA content may be an underlying mechanism of the beneficial effects of breastfeeding on children's metabolism.


Assuntos
Aleitamento Materno/métodos , DNA Mitocondrial/sangue , Doenças Metabólicas/prevenção & controle , Mitocôndrias/metabolismo , Adolescente , Adulto , Estudos de Coortes , Feminino , Humanos , Masculino
20.
Chemosphere ; 242: 125250, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-31896205

RESUMO

Because of their dirt-, water- and oil-repelling properties, per- and polyfluoroalkyl substances (PFASs) are frequently used in a broad variety of consumer products. They have been detected in human samples worldwide. In Flanders, Belgium, the Flemish Environment and Health Studies (FLEHS) measured the levels of five PFAS biomarkers in four different age groups of the Flemish population and identified determinants of variability in exposure. Cord plasma or peripheric serum samples and questionnaire data were available for 220 mother-newborn pairs (2008-2009), 269 mother-newborn pairs (2013-2014), 199 adolescents (14-15 years old, 2010), 201 adults (20-40 years old, 2008-2009) and 205 adults (50-65 years old, 2014). Measured levels of perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorohexane sulfonic acid (PFHxS) and perfluorononanoic acid (PFNA) in Flanders are in the middle or low range compared to concentrations reported in other Western countries. Levels of perfluorobutanesulfonic acid (PFBS) were below the quantification limit in 98%-100% of the samples. Despite decreasing levels in time for PFOS and PFOA, 77% of the adults (2014) had serum levels exceeding HBM-I values of 5 µg/L for PFOS and 2 µg/L for PFOA. Beside age, sex, fish consumption, parity and breastfeeding, the multiple regression models identified additionally consumption of offal and locally grown food, and use of cosmetics as possible exposures and menstruation as a possible route of elimination. Better knowledge on determinants of exposure is essential to lower PFASs exposure.


Assuntos
Exposição Ambiental/estatística & dados numéricos , Poluentes Ambientais/sangue , Adolescente , Adulto , Idoso , Ácidos Alcanossulfônicos/sangue , Bélgica , Aleitamento Materno , Caprilatos/sangue , Saúde Ambiental , Feminino , Fluorocarbonos/sangue , Alimentos , Humanos , Recém-Nascido , Masculino , Pessoa de Meia-Idade , Mães , Paridade , Gravidez , Ácidos Sulfônicos/sangue , Inquéritos e Questionários , Tempo , Adulto Jovem
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