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1.
Molecules ; 25(11)2020 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-32531944

RESUMO

Water from wastewater treatment plants contains concentrations of pharmaceutically active compounds as high as micrograms per liter, which can adversely affect fish health and behavior, and contaminate the food chain. Here, we tested the ability of the common carp hepatic S9 fraction to produce the main metabolites from citalopram, metoprolol, sertraline, and venlafaxine. Metabolism in fish S9 fractions was compared to that in sheep. The metabolism of citalopram was further studied in fish. Our results suggest a large difference in the rate of metabolites formation between fish and sheep. Fish hepatic S9 fractions do not show an ability to form metabolites from venlafaxine, which was also the case for sheep. Citalopram, metoprolol, and sertraline were metabolized by both fish and sheep S9. Citalopram showed concentration-dependent N-desmethylcitalopram formation with Vmax = 1781 pmol/min/mg and Km = 29.7 µM. The presence of ellipticine, a specific CYP1A inhibitor, in the incubations reduced the formation of N-desmethylcitalopram by 30-100% depending on the applied concentration. These findings suggest that CYP1A is the major enzyme contributing to the formation of N-desmethylcitalopram. In summary, the results from the present in vitro study suggest that common carp can form the major metabolites of citalopram, metoprolol, and sertraline.

2.
Anal Bioanal Chem ; 412(18): 4353-4361, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32372276

RESUMO

Recent state-of-the-art methods developed for the analysis of polar xenobiotics from different types of biological matrices usually employ liquid chromatography with mass spectrometry. However, there are limitations when a small amount of sample mass is available. For example, individual benthic invertebrates or fish tissue samples often weigh less than 100 mg (e.g., brain, liver) but are necessary to understand environmental fate and bioaccumulation dynamics. We developed ultra-fast methods based on a direct sample introduction technique. This included coupling laser diode thermal desorption with atmospheric pressure chemical ionization mass spectrometry (LDTD-APCI-MS). We then quantitated a common selective serotonin reuptake inhibitor (citalopram) in brain tissues of individual juvenile fish after in vivo exposure to environmentally relevant concentration. Two mass spectrometric methods based on low (LDTD-APCI-triple quadrupole (QqQ)-MS/MS) and high (LDTD-APCI-high-resolution product scan (HRPS)) resolutions were developed and evaluated. Individual instrument conditions were optimized to achieve an accurate and robust analytical method with minimum sample preparation requirements. We achieved very good recovery (97-108%) across the range of 1-100 ng g-1 for LDTD-APCI-HRPS. LDTD-APCI-QqQ-MS/MS showed poorer performance due to interferences from the matrix at the lowest concentration level. LDTD-APCI ionization was successfully validated for analysis of non-filtered sample extracts. Evaluation of final methods was performed for a set of real fish brain samples, including comparison of LDTD-APCI-HRPS with a previously validated LC-heated electrospray ionization-HRPS method. This new LDTD-APCI-HRPS method avoids the chromatographic step and provides important benefits such as analysis of limited sample masses, lower total sample volume (typically µL), and reduction in analysis time per sample run to a few seconds. Graphical abstract.

3.
Environ Sci Pollut Res Int ; 26(31): 31812-31821, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31487008

RESUMO

Various types of micropollutants, e.g., pharmaceuticals and their metabolites and resistant strains of pathogenic microorganisms, are usually found in hospital wastewaters. The aim of this paper was to study the presence of 74 frequently used pharmaceuticals, legal and illegal drugs, and antibiotic-resistant bacteria in 5 hospital wastewaters in Slovakia and Czechia and to compare the efficiency of several advanced oxidations processes (AOPs) for sanitation and treatment of such highly polluted wastewaters. The occurrence of micropollutants and antibiotic-resistant bacteria was investigated by in-line SPE-LC-MS/MS technique and cultivation on antibiotic and antibiotic-free selective diagnostic media, respectively. The highest maximum concentrations were found for cotinine (6700 ng/L), bisoprolol (5200 ng/L), metoprolol (2600 ng/L), tramadol (2400 ng/L), sulfamethoxazole (1500 ng/L), and ranitidine (1400 ng/L). In the second part of the study, different advanced oxidation processes, modified Fenton reaction, ferrate(VI), and oxidation by boron-doped diamond electrode were tested in order to eliminate the abovementioned pollutants. Obtained results indicate that the modified Fenton reaction and application of boron-doped diamond electrode were able to eliminate almost the whole spectrum of selected micropollutants with efficiency higher than 90%. All studied methods achieved complete removal of the antibiotic-resistant bacteria present in hospital wastewaters.


Assuntos
Ferro/química , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Águas Residuárias/microbiologia , Boro , Cromatografia Líquida , República Tcheca , Diamante , Farmacorresistência Bacteriana , Eletrodos , Hospitais , Peróxido de Hidrogênio/química , Drogas Ilícitas/análise , Resíduos de Serviços de Saúde , Oxirredução , Preparações Farmacêuticas/análise , Eslováquia , Espectrometria de Massas em Tandem , Eliminação de Resíduos Líquidos/instrumentação , Águas Residuárias/análise , Poluentes Químicos da Água/análise
4.
Sci Total Environ ; 669: 983-990, 2019 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-30970465

RESUMO

Organic UV-filters are emergent contaminants continuously released into the aquatic ecosystems. These compounds are persistent showing potential for bioaccumulation. Partial life-cycle tests may underestimate the toxicity of UV-filters especially since these compounds have shown to act as endocrine disruptors. In the present study, the benthic aquatic insect Chironomus riparius was exposed to a gradient of Benzophenone-3 (BP3) concentrations over two generations to assess effects over a full life cycle from the first-instar larvae in the parental (P) generation (emergence, fecundity and fertility) until emergence in the subsequent generation (filial - F1). Recovery from exposure was also assessed after one generational exposure. Our results showed that concentrations of up to 8mg BP3/kg, elicited no effects regarding emergence rate and development time of C. riparius in the P generation. Our results also showed that C. riparius fecundity was not affected by BP3 exposure, but a strong dose-response relationship was observed for fertility with none of the egg ropes hatching at 8mg BP3/kg. Regarding effects observed in the F1 generation, emergence and development time were impaired by continuous exposure to BP3. Moreover, reduced emergence and changes in development time were observed in the F1 generation maintained in control/clean conditions but whose parents were exposed to BP3. Results found in this two-generational study clearly show reproductive effects of BP3 on C. riparius that would not be detected using standard tests. Full life cycle and multigenerational assays are critical to properly evaluate the population level effects of endocrine disrupting compounds such as organic UV-filters.


Assuntos
Benzofenonas/toxicidade , Chironomidae/metabolismo , Disruptores Endócrinos/toxicidade , Protetores Solares/toxicidade , Poluentes Químicos da Água/toxicidade , Animais , Chironomidae/crescimento & desenvolvimento , Relação Dose-Resposta a Droga , Feminino , Fertilidade/efeitos dos fármacos , Larva/crescimento & desenvolvimento , Larva/metabolismo , Masculino
5.
Sci Total Environ ; 659: 326-334, 2019 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-30599351

RESUMO

Drug consumption in individual cities, regions, and at various music events and festivals across the EU has generally been monitored via questionnaires, patients' medical data, and police reports. However, an overview of drug consumption obtained from these methods can be negatively affected by various subjective factors. We aimed to investigate an association between levels of target drugs in wastewater, music genres, and festival courses. The occurrence of illicit drugs, their metabolites, and psychoactive compounds was investigated in the influent of six wastewater treatment plants in the Czech and Slovak Republic during seven large-scale music festivals from different music genres: metal, rock, pop, country and folk, ethnic, multi-genre, dance, and trance. The total number of participants included >130,000 active festival attendees. The association between music genre and illicit drug and/or psychoactive pharmaceutical consumptions is discussed on the basis of the results obtained through wastewater analyses. The observed trend was similar to worldwide published data with a specific local phenomenon of methamphetamine prevalence that did not significantly change between music events. Increased specific loads of cocaine (measured as its metabolite benzoylecgonine) and Ecstasy, along with some cannabis, were mainly observed during pop/rock and dance music festivals. However, there was no significant increase observed in the specific loads of all monitored psychoactive pharmaceuticals. This study demonstrates that the abuse of some illicit drugs is closely associated with specific music preferences.


Assuntos
Monitoramento Ambiental , Férias e Feriados , Drogas Ilícitas/análise , Música , Águas Residuárias/análise , Poluentes Químicos da Água/análise , República Tcheca , Humanos , Eslováquia
6.
Environ Pollut ; 242(Pt A): 417-425, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-29990947

RESUMO

Unknown compounds with (anti-)androgenic activities enter the aquatic environment via municipal wastewater treatment plants (WWTPs). Progestins are well-known environmental contaminants capable of interfering with androgen receptor (AR) signaling pathway. The aim of the present study was to determine if 15 selected progestins have potential to contribute to (anti-)androgenic activities in municipal wastewaters and the respective recipient surface waters. AR-specific Chemically Activated LUciferase gene eXpression bioassay in agonistic (AR-CALUX) and antagonistic (anti-AR-CALUX) modes and liquid chromatography tandem atmospheric pressure chemical ionization/atmospheric photoionization with hybrid quadrupole/orbital trap mass spectrometry operated in high resolution product scan mode (LC-APCI/APPI-HRPS) methods were used to assess (anti-)androgenic activity and to detect the target compounds, respectively. The contribution of progestins to (anti-)androgenic activities was evaluated by means of a biologically and chemically derived toxicity equivalent approach. Androgenic (0.08-59 ng/L dihydrotestosterone equivalents - DHT EQs) and anti-androgenic (2.4-26 µg/L flutamide equivalents - FLU EQs) activities and progestins (0.19-75 ng/L) were detected in selected aquatic environments. Progestins displayed androgenic potencies (0.01-0.22 fold of dihydrotestosterone) and strong anti-androgenic potencies (9-62 fold of flutamide). Although they accounted to some extent for androgenic (0.3-29%) and anti-androgenic (4.6-27%) activities in influents, the progestins' contribution to (anti-)androgenic activities was negligible (≤2.1%) in effluents and surface waters. We also tested joint effect of equimolar mixtures of target compounds and the results indicate that compounds interact in an additive manner. Even if progestins possess relatively strong (anti-)androgenic activities, when considering their low concentrations (sub-ng/L to ng/L) it seems unlikely that they would be the drivers of (anti-)androgenic effects in Czech aquatic environments.


Assuntos
Antagonistas de Androgênios/química , Progestinas/química , Poluentes Químicos da Água/química , Androgênios , Bioensaio/métodos , Águas Residuárias/análise , Águas Residuárias/química , Poluentes Químicos da Água/análise
7.
Sci Total Environ ; 634: 606-615, 2018 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-29635203

RESUMO

The occurrence of 93 pharmaceuticals, illicit drugs and their metabolites has been investigated in stabilized sewage sludge from five municipal wastewater treatment plants (WWTPs) in the Slovak Republic. The total population connected to the tested WWTPs was approximately 600,000 p.e. which represents >20% of the Slovak population connected to public sewer systems. The sludge production from the five tested plants was >8100tons in 2016, which is approximately 15% of the total Slovak sewage sludge production in 2016. The highest total concentration of all pharmaceuticals was found in WWTP Bratislava Devínska Nová Ves (DNV) and Senec - 11,800 and 11,300ng/g dry matter (DM), respectively. Among individual pharmaceuticals, the highest concentrations were recorded for fexofenadine (mean 2340ng/g DM, maximum 5600ng/g DM in Bratislava DNV) and telmisartan (mean 1170ng/g DM, with a maximum of 3370ng/g DM in Senec). A principal component analysis revealed differences between pharmaceutical patterns in aerobically and anaerobically stabilized sludge. The worst-case scenario based on no further degradation of pharmaceuticals between sludge production and field application was used to predict pharmaceutical mass loads in agriculture. For the result, we estimated an annual load to soil in the Slovak Republic of up to several hundred kilograms of pharmaceuticals and drugs, with the maximum for fexofenadine (120kg/year) and verapamil (29kg/year).

8.
J Chromatogr A ; 1392: 110-7, 2015 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-25818560

RESUMO

Some potential problems that can occur during the analyses of complex samples by on-line combination of capillary isotachophoresis-capillary zone electrophoresis (cITP-CZE) in automated electrophoretic analyzer with the column-coupling configuration of the separation unit were studied in this work. The main focus was devoted on the reproducibility of important analytes' parameters (migration time, peak height and peak area) and also on the stability studies of selected low and high molecular mass analytes of inorganic/organic origins (bromate, vitamins, proteins) present at low concentration levels in different kinds of matrices (mineral water, human urine). Such study was carried out for the first time for the electrophoretic analyzer operating in the hydrodynamically closed separation system provided with contact-less conductivity detectors and UV detector in CZE step. Hydrodynamic and electroosmotic flows of the buffer solutions were suppressed and therefore, only the electrophoretic transport of ions was significant. Obtained results showed the different stabilities of the analytes and samples depending on their origin. The focus in the long-term analyses should be paid on the storage of the samples and on the regular changing the contents of electrolyte vessels to keep the electrolyte composition and separation conditions as constant as possible.


Assuntos
Eletroforese Capilar/métodos , Bromatos/análise , Eletro-Osmose , Humanos , Hidrodinâmica , Isotacoforese , Águas Minerais/análise , Muramidase/análise , Proteínas/análise , Reprodutibilidade dos Testes , Albumina Sérica/análise , Urinálise , Vitamina B 6/análise
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