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See detailSelection and ranking method for currently used pesticides (CUPs) monitoring in ambient air
Giusti, Arnaud; PIRARD, Catherine ULiege; CHARLIER, Corinne ULiege et al

in Air Quality, Atmosphere and Health (2018)

Chronic exposure to pesticides can induce adverse human health effects. Even though ingestion is considered as the main exposure pathway, it is now suggested that inhalation might also be important not ... [more ▼]

Chronic exposure to pesticides can induce adverse human health effects. Even though ingestion is considered as the main exposure pathway, it is now suggested that inhalation might also be important not only in rural but also in urban locations. Therefore, assessment of currently used pesticides (CUPs) concentrations in ambient air is important for better understanding of human exposure through inhalation and potential health effects. Analytical methods do not allow assessing ambient air concentration of all the CUPs registered. Designing a cost-effective and a fitted-for-purpose monitoring strategy at the local/regional scale must therefore rely on a methodology allowing targeting CUPs by a ranking approach accounting for the most relevant selection criteria. In this study, after a first selection, a ranking method is used to identify most relevant CUPs for ambient air assessment in Wallonia, Belgium. This method took into account not only toxicological endpoints but also national and regional data on sales and uses along with other uses criteria. Moreover, probability to detect CUPs in ambient air was investigated using international, national, and regional studies and physicochemphysicochemical properties. The ranking method used three main criteria (i.e., chronic toxicity, sales and uses, and presence in ambient air), which are divided in 17 sub-criteria, to provide the most accurate identification of CUPs that might be measured in ambient air and that might impact human health. After final selection based on analytical methods, 43 CUPs were further submitted to analytical method development. [less ▲]

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See detailAssociation between organohalogenated pollutants in cord blood and thyroid function in newborns and mothers from Belgian population
Dufour, Patrice ULiege; PIRARD, Catherine ULiege; Seghaye, Marie-Christine ULiege et al

in Environmental Pollution (2018), 238

The last decades have seen the increasing prevalence of thyroid disorders. These augmentations could be the consequence of the increasing contamination of the environment by chemicals that may disrupt the ... [more ▼]

The last decades have seen the increasing prevalence of thyroid disorders. These augmentations could be the consequence of the increasing contamination of the environment by chemicals that may disrupt the thyroid function. Indeed, in vitro studies have shown that many chemicals contaminating our environment and highlighted in human serum, are able to interfere with the thyroid function. Given the crucial importance of thyroid hormones on neurodevelopment in fetus and newborns, the influence of these pollutants on newborn thyroid homeostasis is a major health concern. Unfortunately, the overall evidence for a deleterious influence of environmental pollutants on thyroid remains poorly studied. Therefore, we assessed the contamination by polychlorinated biphenyls (PCBs), organochlorine pesticides and perfluorinated compounds (PFC) in 221 cord blood samples collected in Belgium between 2013 and 2016. Our results showed that compared to previous studies performed on newborns recruited in Belgium during the two last decades, the present pollutant contamination is declining. Multivariate statistical analyses pointed out a decrease of thyroid stimulating hormone (TSH) level in male newborns with detectable level of 4,40- dichlorodiphenyldichloroethylene (4,40-DDE) in comparison with those with no detectable level (p ¼ 0.025). We also highlighted a negative association between perfluorononanoic acid (PFNA) concentration and TSH in male newborns (p ¼ 0.018). Logistic regression showed increased odds ratio for presentation of hypothyroid in mother for each one unit augmentation of log natural concentration of PFOA (OR ¼ 2.30, [1.18e4.5]) and PFOS (OR ¼ 2.03 [1.08e3.83]). Our findings showed that the residual contamination by PFCs and organochlorine pollutants in cord blood are correlated with thyroid hormone in the newborns and the risk of hypothyroid in mothers. [less ▲]

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See detailThe current environmental levels of endocrine disruptors (mercury, cadmium, organochlorine pesticides and PCBs) in a Belgian adult population and their predictors of exposure
PIRARD, Catherine ULiege; Compere, Stéphanie; Firquet, Cathy et al

in International Journal of Hygiene and Environmental Health (2018), 221

A human biomonitoring study was carried out measuring the levels of endocrine disruptors in 252 participants (18-76 years old) recruited between February and May 2015 from the general population of Liege ... [more ▼]

A human biomonitoring study was carried out measuring the levels of endocrine disruptors in 252 participants (18-76 years old) recruited between February and May 2015 from the general population of Liege Province (Belgium). In this study, we reported the recent levels of cadmium and mercury in urine, some organochlorine pesticides and polychlorinated biphenyls (PCBs) in serum, and their relations to demographic characteristics, lifestyle behaviors and dietary habits. The median urinary levels of mercury and cadmium were 0.81 µg/l and <0.5µg/l respectively. The mercury levels were higher in participants having at least 3 dental amalgams, and consuming sea fish more than once a week. Although our mercury levels in most participants were lower than some health-based guidelines, they were higher than in our neighboring countries where ban or restrictions on the dental amalgams use were implemented. Urinary cadmium levels in current smokers were significantly higher than former or never smokers, as well as non-smokers for passively exposed vs non-exposed ones. Median PCB-153 and -180 serum levels were 53.8 and 41.1 ng/g lipid respectively, but PCB-138 was below the limit of quantification of 0.15 µg/l in 49% of the samples. Among the organochlorine pesticides, 4,4’-dichlorodiphenyldichloroethylene (4,4’-DDE), beta-hexachlorohexane and hexachlorobenzene were positively detected respectively in 48%, 49% and 37% of the serum samples. Eventhough, a dramatic decrease in organochlorines levels was observed, at least 1 pesticide or PCB was detected in 96% of our population, and more than 50% of our samples were contaminated by 4 or more organochlorines. Age, body mass index, and breastfeeding duration were the most predictive determinants of pesticide or PCB serum concentrations, but not dietary habits. [less ▲]

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See detailDetermination of phenolic organohalogens in human serum from a Belgian population and assessment of parameters affecting the human contamination
Dufour, Patrice ULiege; PIRARD, Catherine ULiege; CHARLIER, Corinne ULiege

in Science of the Total Environment (2017), 599-600

Many in vitro or in vivo studies highlighted the potential deleterious effects of phenolic organohalogenated compounds (POHs) on the health, particularly on the thyroid system homeostasis, however few ... [more ▼]

Many in vitro or in vivo studies highlighted the potential deleterious effects of phenolic organohalogenated compounds (POHs) on the health, particularly on the thyroid system homeostasis, however few large scale human epidemiological studies have been carried out, especially in Europe. Further studies monitoring the human contamination by POHs, the sources of exposure and the influence of these compounds on thyroid health are still needed. Therefore we determined the concentrations of 16 POHs (pentachlorophenol (PCP), tetrabromobisphenol A (TBBPA), 4 bromophenols (BPs), 3 hydroxy-polybromodiphenylethers (OH-PBDEs) and 7 hydroxy-polychlorobiphenyls (OH-PCBs)) in serum from 274 people aged from 18 to 76 years old living in Liege (Belgium) and the surrounding area. A questionnaire about their alimentary habits, life style and home environment was also administered to the volunteers. The predominant compound measured in the population was PCP (median concentration of 593.0 pg mL−1). 4-OH-CB 107, 4-OH-CB 146 and 4-OH-CB 187 were detected in all samples and contributed for 75% of the sum of OH-PCBs (ΣOH-PCBs). The median measured in our population for ΣOH-PCBs was 143.7 pg mL−1. TBBPA and 2,4,6-tribromophenol were detected in 31% and 63.8% of the samples respectively while the detection frequency observed for the other BPs and the OH-PBDEs was close to zero. We computed multivariate regression models in order to assess the influence of demographic and lifestyle parameters on the PCP and ΣOH-PCBs contamination levels. Significant correlation was found between the PCP concentration and sex, smoker status, sea fish consumption and level of education, although the model seemed to be a poor (R2 = 0.14) predictor of the PCP concentration. The model computed for ΣOHPCBs was more explanatory (R2 = 0.61) and involved age, BMI and sea fish consumption. Finally, we assessed the parameters affecting the ΣOH-PCBs/ΣPCBs ratio. The model proposed involved age, BMI, smoker status and parent PCB level, and explained 41% of the variability of the ΣOH-PCBs/ΣPCBs ratio. [less ▲]

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See detailDetermination of polybrominated diphenyl ethers and some novel brominated flame retardants in a Belgian population
PIRARD, Catherine ULiege; Dozot, Guillaume ULiege; Charlier, Corinne ULiege

Poster (2017, October)

Aims Brominated flame retardants (BFRs) were widely used these past decades in textiles, plastics, electric or electronic equipments, etc, to prevent or reduce the ignition and rate of combustion. Due to ... [more ▼]

Aims Brominated flame retardants (BFRs) were widely used these past decades in textiles, plastics, electric or electronic equipments, etc, to prevent or reduce the ignition and rate of combustion. Due to their persistence and health concerns, the production and uses of several BFRs were banned in many countries. Recently, emerging BFRs have been developed as alternatives to the banned or restricted chemicals, but data on their human exposure are still scarce. The aims of this study were firstly to develop and validate a fast and simple analytical procedure to measure 15 historical and novel BFRs in human serum, allowing high throughput analyses for large scale epidemiological studies. Secondly, this new method was used to assess the environmental exposure of a general population living in the Province of Liege (Belgium). Materials and Methods 1 ml of serum previously equilibrated for 1 hour with internal standard and acetic acid glacial was extracted twice using a hexane/acetone mixture (95/5). After evaporation till 0.5ml, the extract was loaded on 1ml PHREE cartridge (Phenomenex) to remove lipid traces, and transferred to GC vial with nonane as keeper. The final determination was performed on a gas chromatograph (GC) coupled to a mass spectrometer (7890A GC/7000A Triple Quad MS, Agilent Technologies), and equipped with a 15 meters RTX-1614 (Restek). The MS operated in Negative Chemical ionization mode using methane as reagent gas. 252 volunteers living in the Province of Liege (Belgium) were recruited between February and May 2015 from the High Schools and Provincial Offices, and provided urine and blood samples. From this enrollment, the serum of 43 participants aged from 18 to 29 years old, and 50 aged from 40 to 49 years were analyzed for BFRs. Results and Conclusions The fast extraction procedure provided clean extracts and good recovery rates from small serum volume and did not need further labor and time consuming purification steps. The 15m length RTX-1614 allowed the simultaneous measurement of the 15 BFRs including PBDE-209 in a single injection. From the 15 initial targeted BFRs, 8 PBDEs including PBDE-209, 1 hexabromobiphenyl (PBB-153), pentabromotoluene (PBT), hexabromobenzene (HxBBz), and pentabromoethylbenzene (PBEB) were successfully validated according the total error approach. This user-friendly method was demonstrated to be accurate, exact, and could be easily implemented in routine laboratories. The limit of quantification was defined at 47.2 pg/ml for PBDE-209, the others ranging from 1 to 9.2 pg/ml. Within the population studied, all targeted BFRs were measured with detection frequencies (DF) ranging from 2.2 to 39.8%, except for PBDE-183 and PBEB which were never detected. The most often found BFRs were successively PBDE-153, -154, -47, -100 and -99. The geometric means ranged between 0.11 and 3.81 ng/g lipid depending on the compound, which were far lower than levels usually reported in North America or in China (1). Women showed significantly higher DF than men for PBDE-47, -99, -100 but lower for PBDE-153, suggesting different metabolism efficiency or different pollutant storage according to gender. On the other hand, the older age class (40-49 yr) showed higher DF only for PBB-153 and PBDE-154. References : (1) Zhu et al., Brominated Flame Retardants in serum from the general population in Nothern China. Environ. Sci. Technol. 2009, 43 (18): 6963-6968 [less ▲]

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See detailBiocompatibility of polymer-infiltrated-ceramicnetwork (PICN) materials with Human Gingival Keratinocytes (HGKs)
GRENADE, Charlotte ULiege; Gillet, Marie-Claire ULiege; PIRARD, Catherine ULiege et al

in Dental Materials (2017), 33

Objective. Biocompatibility of polymer-infiltrated-ceramic-network (PICN) materials, a new class of CAD–CAM composites, is poorly explored in the literature, in particular, no data are available regarding ... [more ▼]

Objective. Biocompatibility of polymer-infiltrated-ceramic-network (PICN) materials, a new class of CAD–CAM composites, is poorly explored in the literature, in particular, no data are available regarding Human Gingival Keratinocytes (HGK). The first objective of this study was to evaluate the in vitro biocompatibility of PICNs with HGKs in comparison with other materials typically used for implant prostheses. The second objective was to correlate results with PICN monomer release and indirect cytotoxicity. Methods. HGK attachment, proliferation and spreading on PICN, grade V titanium (Ti), yttrium zirconia (Zi), lithium disilicate glass-ceramic (eM) and polytetrafluoroethylene (negative control) discs were evaluated using a specific insert-based culture system. For PICN and eM samples, monomer release in the culture medium was quantified by high performance liquid chromatography and indirect cytotoxicity tests were performed. Results. Ti and Zi exhibited the best results regarding HGK viability, number and coverage. eM showed inferior results while PICN showed statistically similar results to eM but also to Ti regarding cell number and to Ti and Zi regarding cell viability. No monomer release from PICN discs was found, nor indirect cytotoxicity, as for eM. Significance. The results confirmed the excellent behavior of Ti and Zi with gingival cells. Even if polymer based, PICN materials exhibited intermediate results between Ti–Zi and eM. These promising results could notably be explained by PICN high temperature–high pressure (HT–HP) innovative polymerization mode, as confirmed by the absence of monomer release and indirect cytotoxicity [less ▲]

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See detailA Simple Tiered Methodology for the Determination of Ambient Air Quality Guidelines
PIRARD, Catherine ULiege; Brouhon, Jean-Marc; Fourmeaux, Annick et al

in Clean : Soil, Air, Water (2016), 44(5), 464-473

Within the scope of the renewal of industrial operating permits in Belgium, the Walloon Agency for Air and Climate needed air quality criteria for a wide range of toxics. Due to the plethora of different ... [more ▼]

Within the scope of the renewal of industrial operating permits in Belgium, the Walloon Agency for Air and Climate needed air quality criteria for a wide range of toxics. Due to the plethora of different existing values for some compounds or the total lack for others, the development of a simple methodology was required to provide both quality and intervention criteria, corresponding respectively to a chemical concentration for which no adverse health effects are expected for a lifetime exposure, and the chemical concentration in air associated with a risk for human health deemed significant. The tiered methodology developed here allows the selection of air guidelines from available databases, and proposes, if needed, approaches based on well-proven procedures to derive air quality guidelines from occupational exposure limits, drinking water guidelines, tolerable daily intakes, or as a last resort acute lethal toxicity data if nothing else is available. If this method has been successfully applied to more than 550 compounds, all values produced should be validated according to the purpose of the guidelines, the technical feasibility of achieving the threshold produced, and the specificity of the environment conditions and the targeted population. Moreover, the criteria obtained from non-air-related data should be critically examined and handled with caution. [less ▲]

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See detailValidation of a novel and rapid method for simultaneous determination of some phenolic organohalogens in serum by GC-MS
Dufour, Patrice ULiege; PIRARD, Catherine ULiege; Charlier, Corinne ULiege

in Journal of Chromatography. B : Analytical Technologies in the Biomedical & Life Sciences (2016), 1036

Over the last decades, more and more studies focused on the impact of endocrine disruptors on the environment and human health. Among them, phenolic organohalogens (POHs) are a particular concern because ... [more ▼]

Over the last decades, more and more studies focused on the impact of endocrine disruptors on the environment and human health. Among them, phenolic organohalogens (POHs) are a particular concern because of their structural resemblance with natural hormones. There are different methods that are known to quantify these compounds in human serum, however, the current extraction techniques are long, fastidious and using harmfull chemicals such as diazomethane and sulfuric acid. Consequently, we developed an alternative, sensitive and faster method to simultaneously quantify pentachlorophenol (PCP), tetrabromobisphenol A (TBBPA), 4 bromophenols, 7 hydroxypolychlorinated biphenyls (OH-PCBs) and 3 hydroxy-polybrominated diphenyl ether (OH-PBDEs) in human serum sample. The clean-up and the enrichment of the sample were performed in a single extraction step using strong anion-exchange solid phase cartridge. After a rapid liquid–liquid extraction step to remove acidic traces, the extract was derivatized using trimethylsilyldiazomethane (TMSD) and finally analyzed by a gas-chromatograph coupled with an electron negative capture chemical ionization source combined with a triple quadrupole mass spectrometer (GC-ENCI-MS) operating in single ion monitoring. The whole procedure was validated according to the total error approach. The inter and intra assay precision were demonstrated to be lower than 20% and the relative bias to be lower than 15% in the dosing range of concentrations. The limit of quantification (LOQ) ranged from 2 pg mL−1 and 5 pg mL−1, except for the PCP (44.6 pg mL−1) and for the 2,4,6-tribromophenol (49.6 pg mL−1). Finally, the method was successfully applied to measure the POH background contamination in serum samples collected from 20 Belgian blood donors recruited in CHU Mont-Godinne (Namur, Belgium) aged between 21 and 69 years old. [less ▲]

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See detailA Simple tiered methodology for the determination of ambient air quality guidelines
PIRARD, Catherine ULiege; DUBOIS, Nathalie ULiege; BROUHON, Jean-Marc et al

Poster (2015, November)

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See detailTemporal variability of urinary concentrations of phthalate metabolites, parabens and benzophenone-3 in a belgian adult population
DEWALQUE, Lucas ULiege; PIRARD, Catherine ULiege; Vandepaer, Sarah et al

in Environmental Research (2015), 142

In the present study, we investigated the temporal within-person variability of the exposure biomarker for phthalates, parabens and benzophenone-3 (BP3) in 32 Belgian adults, each providing 11 urine spots ... [more ▼]

In the present study, we investigated the temporal within-person variability of the exposure biomarker for phthalates, parabens and benzophenone-3 (BP3) in 32 Belgian adults, each providing 11 urine spots during 4 months. We calculated the intraclass coefficient correlation (ICC), the sensitivity and the specificity to assess the temporal reproducibility and to investigate the predictive ability of the spot measurements for these classes of chemicals. Additionally, we explored the temporal variability of the estimation of the cumulative risk of exposure to phthalates (hazard index; HI). We observed fair ICC ranging from 0.55 to 0.68 for parabens, monoethyl phthalate (MEP), mono-iso-butyl phthalate (MiBP) and BP3, but lower ICC, from 0.20 to 0.49, for monobenzyl phthalate (MBzP), mono-n-butyl phthalate (MnBP), mono-2-ethylhexyl phthalate (MEHP), mono-2-ethyl-5-oxo-hexyl phthalate (5-oxo-MEHP) and mono-2-ethyl-5-hydroxy-hexyl phthalate (5-OH-MEHP). The ICC estimated for HI (0.49) reflected a moderate reproducibility. The measurements in spot samples were moderate to good predictor of the 4-month level of exposure for parabens, MEP, MnBP, MiBP, BP3 and HI (sensitivity ranging from 0.67 to 0.77), but lower predictor for MEHP, 5-oxo-MEHP, 5-OH-MEHP and MBzP (sensitivity ranging from 0.58 to 0.63). The sensitivity could be increased when several spot urinary levels were averaged to predict the long-term level of exposure. Globally, our results indicate that a single spot measurement seems to correctly represent the long-term exposure for parabens, BP3, MEP, MiBP and HI. Additional spot samples seemed to be needed for the proper exposure assessment of the other target compounds. [less ▲]

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See detailFish consumption patterns and hair mercury levels in children and their mothers in 17 EU countries
Castano, Argelia; Cutanda, Francisco; Esteban, Marta et al

in Environmental Research (2015), 141

The toxicity of methylmercury (MeHg) in humans is well established and the main source of exposure is via the consumption of large marine fish and mammals. Of particular concern are the potential ... [more ▼]

The toxicity of methylmercury (MeHg) in humans is well established and the main source of exposure is via the consumption of large marine fish and mammals. Of particular concern are the potential neurodevelopmental effects of early life exposure to low-​levels of MeHg. Therefore, it is important that pregnant women, children and women of childbearing age are, as far as possible, protected from MeHg exposure. Within the European project DEMOCOPHES, we have analyzed mercury (Hg) in hair in 1799 mother-​child pairs from 17 European countries using a strictly harmonized protocol for mercury anal. Parallel, harmonized questionnaires on dietary habits provided information on consumption patterns of fish and marine products. After hierarchical cluster anal. of consumption habits of the mother-​child pairs, the DEMOCOPHES cohort can be classified into two branches of approx. similar size: one with high fish consumption (H) and another with low consumption (L)​. All countries have representatives in both branches, but Belgium, Denmark, Spain, Portugal and Sweden have twice as many or more mother-​child pairs in H than in L. For Switzerland, Czech Republic, Hungary, Poland, Romania, Slovenia and Slovakia the situation is the opposite, with more representatives in L than H. There is a strong correlation (r=0.72) in hair mercury concn. between the mother and child in the same family, which indicates that they have a similar exposure situation. The clustering of mother-​child pairs on basis of their fish consumption revealed some interesting patterns. One is that for the same sea fish consumption, other food items of marine origin, like seafood products or shellfish contribute significantly to the mercury levels in hair. We conclude that addnl. studies are needed to assess and quantify exposure to mercury from seafood products, in particular. The cluster anal. also showed that 95​% of mothers who consume once per wk fish only, and no other marine products, have mercury levels 0.55 μg​/g. Thus, the 95th percentile of the distribution in this group is only around half the US-​EPA recommended threshold of 1 μg​/g mercury in hair. Consumption of freshwater fish played a minor role in contributing to mercury exposure in the studied cohort. The DEMOCOPHES data shows that there are significant differences in MeHg exposure across the EU and that exposure is highly correlated with consumption of fish and marine products. Fish and marine products are key components of a healthy human diet and are important both traditionally and culturally in many parts of Europe. Therefore, the communication of the potential risks of mercury exposure needs to be carefully balanced to take into account traditional and cultural values as well as the potential health benefits from fish consumption. European harmonized human biomonitoring programs provide an addnl. dimension to national HMB programs and can assist national authorities to tailor mitigation and adaptation strategies (dietary advice, risk communication, etc.) to their country's specific requirements. [less ▲]

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See detailMercury analysis in hair: Comparability and quality assessment within the transnational COPHES/DEMOCOPHES project
Esteban, Marta; Schindler, Birgit K.; Jiménez-Guerrero, José A. et al

in Environmental Research (2015), 141

Human biomonitoring (HBM) is an effective tool for assessing actual exposure to chemicals that takes into account all routes of intake. Although hair analysis is considered to be an optimal biomarker for ... [more ▼]

Human biomonitoring (HBM) is an effective tool for assessing actual exposure to chemicals that takes into account all routes of intake. Although hair analysis is considered to be an optimal biomarker for assessing mercury exposure, the lack of harmonization as regards sampling and analytical procedures has often limited the comparison of data at national and international level. The European-funded projects COPHES and DEMOCOPHES developed and tested a harmonized European approach to Human Biomonitoring in response to the European Environment and Health Action Plan. Herein we describe the quality assurance program (QAP) for assessing mercury levels in hair samples from more than 1800 mother–child pairs recruited in 17 European countries. To ensure the comparability of the results, standard operating procedures (SOPs) for sampling and for mercury analysis were drafted and distributed to participating laboratories. Training sessions were organized for field workers and four external quality-assessment exercises (ICI/EQUAS), followed by the corresponding web conferences, were organized between March 2011 and February 2012. ICI/EQUAS used native hair samples at two mercury concentration ranges (0.20–0.71 and 0.80–1.63) per exercise. The results revealed relative standard deviations of 7.87–13.55% and 4.04–11.31% for the low and high mercury concentration ranges, respectively. A total of 16 out of 18 participating laboratories the QAP requirements and were allowed to analyze samples from the DEMOCOPHES pilot study. Web conferences after each ICI/EQUAS revealed this to be a new and effective tool for improving analytical performance and increasing capacity building. The procedure developed and tested in COPHES/DEMOCOPHES would be optimal for application on a global scale as regards implementation of the Minamata Convention on Mercury. [less ▲]

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See detailChapter 4 : Human Exposure of Bisphenol A : Review of the Urinary Levels in the General Population
PIRARD, Catherine ULiege; Charlier, Corinne ULiege

in Gibert, Yann (Ed.) Bisphenol A : Sources, Risks of Environmental Exposure and Human Health Effects (2015)

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