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1.
Environ Pollut ; : 116121, 2020 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-33272798

RESUMO

POCIS is the most widely applied passive sampler of polar organic substances, because it was one of the first commercially available samplers for that purpose on the market, but also for its applicability for a wide range of substances and conditions. Its main weakness is the variability of sampling performance with exposure conditions. In our study we took a pragmatic approach and performed in situ calibration for a set of 76 pharmaceuticals and their metabolites in five sampling campaigns in surface water, covering various temperature and flow conditions. In individual campaigns, RS were calculated for up to 47 compounds ranging from 0.01 to 0.63 L d-1, with the overall median value of 0.10 L d-1. No clear changes of RS with water temperature or discharge could be found for any of the investigated substances. The absence of correlation of experimental RS with physical-chemical properties in combination with the lack of mechanistic understanding of compound uptake to POCIS implies that practical estimation of aqueous concentrations from uptake in POCIS depends on compound-specific experimental calibration data. Performance of POCIS was compared with grab sampling of water in seven field campaigns comprising multiple sampling sites, where sampling by both methods was done in parallel. The comparison showed that for 25 of 36 tested compounds more than 50% of POCIS-derived aqueous concentrations did not differ from median of grab sampling values more than by a factor of 2. Further, for 30 of 36 compounds, more than 80% of POCIS data did not differ from grab sampling data more than by a factor of 5. When accepting this level of accuracy, in situ derived sampling rates are sufficiently robust for application of POCIS for identification of spatial and temporal contamination trends in surface waters.

2.
Environ Int ; 138: 105597, 2020 05.
Artigo em Inglês | MEDLINE | ID: mdl-32120059

RESUMO

The occurrence of chemical and biological contaminants of emerging concern (CECs) was investigated in treated wastewater intended for reuse in agriculture. An agarose hydrogel diffusion-based passive sampler was exposed to the outlet of a wastewater treatment plant (WWTP) located in Cyprus, which is equipped with membrane bioreactor (MBR). Passive samplers in triplicate were exposed according to a time-series exposure plan with maximum exposure duration of 28 days. Composite flow-proportional wastewater samples were collected in parallel with the passive sampling exposure plan and were processed by solid phase extraction using HORIZON SPE-DEX 4790 and the same sorbent material (Oasis HLB) as in the passive sampler. The analysis of passive samplers and wastewater samples enabled (i) the field-scale calibration of the passive sampler prototype by the calculation of in situ sampling rates of target substances, and (ii) the investigation of in silico predicted transformation products of the four most ecotoxicologically hazardous antibiotics (azithromycin, clarithromycin, erythromycin, ofloxacin). Additionally, the wastewater samples were subjected to the analysis of seven preselected antibiotic resistant genes (ARGs) and one mobile resistant element (int1). All extracts were analyzed for chemicals in a single batch using a highly sensitive method for pharmaceuticals, antibiotics and illicit drugs by liquid chromatography tandem MS/MS (LC-QQQ) and for various other target compounds (2316 compounds in total) by liquid chromatography high-resolution mass spectrometry (LC-HRMS). 279 CECs and all investigated ARGs (except for blaCTX-M-32) were detected, highlighting potential chemical and biological hazards related to wastewater reuse practices. 16 CECs were prioritized following ecotoxicological risk assessment, whereas sul1 and the mobile resistant element (int1) showed the highest abundance. Comprehensive monitoring efforts using novel sampling methods such as passive sampling, wide-scope target screening and molecular analysis are required to assure safe application of wastewater reuse and avoid spread and crop uptake of potentially hazardous chemicals.


Assuntos
Águas Residuárias , Poluentes Químicos da Água , Agricultura , Monitoramento Ambiental , Espectrometria de Massas em Tandem , Poluentes Químicos da Água/análise
3.
Sci Total Environ ; 720: 137480, 2020 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-32146393

RESUMO

Silicone (polydimethylsiloxane or PDMS) wristbands and cotton T-shirts were used to assess the exposure of e-waste recyclers in Dhaka, Bangladesh to polybrominated diphenyl ethers (PBDEs), novel brominated flame retardants (NBFRs), dechlorane plus (DPs), and organophosphate esters (OPEs). The median surface-normalized uptake rates of PBDEs, NBFRs, DPs, and OPEs were 170, 8.5, 4.8, and 270 ng/dm2/h for wristbands and 5.4, 2.0, 0.94, and 23 ng/dm2/h for T-shirts, respectively. Concentrations of Tris(2-chloroethyl) phosphate (TCEP), Tris(1,3-dichloro-2-propyl) phosphate (TDCIPP), Tri-m-cresyl phosphate (TmCP), Bis(2-ethlyhexyl) tetrabromophthalate (BEH-TEBP), and Dechlorane plus (DPs) in wristbands were significantly correlated with those in T-shirts. Wristbands accumulated ~7 times more mass than T-shirts, especially of compounds expected to be mainly in the gas phase. We introduce the silicone "sandwich" method to approximate the easily releasable fraction (ERF) from T-shirts, hypothesized to be related to dermal exposure. ERFs varied from 6 to 75% of total chemical accumulated by T-shirts and were significantly negatively correlated with compounds' octanol-air partition coefficient (log Koa). The median daily exposure doses via dermal transfer from the front of the T-shirt to the front body trunk were 0.32, 0.13, 0.11, and 9.1 ng/kg-BW/day for PBDEs, NBFRs, DPs, and OPEs, respectively. The evidence of e-waste recycler exposure to flame retardants in this low income country, lacking protective personal equipment, calls for measures to minimize their exposure and for chemical management regulations to consider exposures to chemicals in waste products.


Assuntos
Resíduo Eletrônico , Bangladesh , Monitoramento Ambiental , Ésteres , Retardadores de Chama , Éteres Difenil Halogenados , Organofosfatos , Silicones
4.
Chemosphere ; 249: 126183, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32088466

RESUMO

Diffusion coefficient (D) is an important parameter for prediction of micropollutant uptake kinetics in passive samplers. Passive samplers are nowadays commonly used for monitoring trace organic pollutants in different environmental matrices. Samplers utilising a hydrogel layer to control compound diffusion are gaining popularity. In this work we investigated diffusion of several perfluoroalkyl substances, currently used pesticides, pharmaceuticals and personal care products in 1.5% agarose hydrogel by measuring diffusion coefficients using two methods: a diffusion cell and a sheet stacking technique. Further, diffusion coefficients in water were measured using Taylor dispersion method. The sheet stacking method was used to measure D at 5, 12, 24, and 33 °C in order to investigate temperature effect on diffusion. Median D values ranged from 2.0 to 8.6 × 10-6 cm2 s-1 and from 2.1 to 8.5 × 10-6 cm2 s-1 for the diffusion cell and sheet stack methods respectively. For most compounds, the variability between replicates was higher than the difference between values obtained by the two methods. Rising temperature from 10 to 20 °C increases the diffusion rate by the factor of 1.41 ± 0.10 in average. In water, average D values ranged from 3.03 to 10.0 × 10-6 cm2 s-1 and were comparable to values in hydrogel, but some compounds including perfluoroalkyl substances with a long aliphatic chain could not be evaluated properly due to sorptive interactions with capillary walls in the Taylor dispersion method. Sampling rates estimated using the measured D values were systematically higher than values estimated from laboratory sampler calibration in our previously published study, by the factor of 2.2 ± 1.0 in average.


Assuntos
Monitoramento Ambiental/métodos , Sefarose/análise , Poluentes Químicos da Água/análise , Transporte Biológico , Cosméticos , Difusão , Monitoramento Ambiental/instrumentação , Hidrogéis , Cinética , Compostos Orgânicos , Praguicidas/análise , Temperatura , Água
5.
Environ Sci Pollut Res Int ; 26(15): 15273-15284, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30929173

RESUMO

Passive samplers based on diffusive gradients in thin hydrogel films (DGT) were recently modified for sampling of polar organic compounds in water. However, since the sampling rates of the commonly used DGT design with the surface area of 3.1 cm2 are low, we propose to increase them by applying a two-sided design with a larger sampling surface area of 22.7 cm2. The sampler design consists of two sorptive hydrogel disks compressed between two diffusive hydrogel disk layers strengthened by nylon netting and held together by two stainless steel rings. Sorbent/water distribution coefficients (KSW) were determined, and the sampler was calibrated for monitoring 11 perfluoroalkyl substances and 12 pharmaceuticals and personal care products in water at laboratory conditions using a closed system with artificial flow generated by submersible pumps. A field performance test was conducted at five locations in the Morava River basin in Czech Republic. The median value of laboratory-derived sampling rates was 43 mL day-1 with extreme values of 2 mL day-1 and 90 mL day-1 for perfluorotridecanoic and perfluoroheptanoic acids, respectively. The log KSW values of tested compounds ranged from 3.18 to 5.47 L kg-1, and the estimated halftime to attain sampler-water equilibrium ranged from 2 days to more than 28 days, which is the maximum recommended exposure period, considering potential issues with the stability of hydrogel. The sampler can be used for assessment of spatial trends as well as estimation of aqueous concentration of investigated polar compounds.


Assuntos
Fluorcarbonetos/química , Ácidos Heptanoicos/química , Hidrogéis/química , Compostos Orgânicos/química , Sefarose/química , Poluentes Químicos da Água/análise , República Tcheca , Difusão , Rios/química , Água
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