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Novel pollutants in the Moscow atmosphere in winter period: Gas chromatography-high resolution time-of-flight mass spectrometry study
2017
Mazur, D.M. | Polyakova, O.V. | Artaev, V.B. | Lebedev, A.T.
The most common mass spectrometry approach analyzing contamination of the environment deals with targeted analysis, i.e. detection and quantification of the selected (priority) pollutants. However non-targeted analysis is becoming more often the method of choice for environmental chemists. It involves implementation of modern analytical instrumentation allowing for comprehensive detection and identification of the wide variety of compounds of the environmental interest present in the sample, such as pharmaceuticals and their metabolites, musks, nanomaterials, perfluorinated compounds, hormones, disinfection by-products, flame retardants, personal care products, and many others emerging contaminants. The paper presents the results of detection and identification of previously unreported organic compounds in snow samples collected in Moscow in March 2016. The snow analysis allows evaluation of long-term air pollution in the winter period. Gas chromatography coupled to a high resolution time-of-flight mass spectrometer has enabled us with capability to detect and identify such novel analytes as iodinated compounds, polychlorinated anisoles and even Ni-containing organic complex, which are unexpected in environmental samples. Some considerations concerning the possible sources of origin of these compounds in the environment are discussed.
Afficher plus [+] Moins [-]Antimicrobial activity of pharmaceutical cocktails in sewage treatment plant effluent – An experimental and predictive approach to mixture risk assessment
2017
Menz, Jakob | Baginska, Ewelina | Arrhenius, Åsa | Haiß, Annette | Backhaus, Thomas | Kümmerer, Klaus
Municipal wastewater contains multi-component mixtures of active pharmaceutical ingredients (APIs). This could shape microbial communities in sewage treatment plants (STPs) and the effluent-receiving ecosystems. In this paper we assess the risk of antimicrobial effects in STPs and the aquatic environment for a mixture of 18 APIs that was previously detected in the effluent of a European municipal STP. Effects on microbial consortia (collected from a separate STP) were determined using respirometry, enumeration of culturable microorganisms and community-level physiological profiling. The mixture toxicity against selected bacteria was assessed using assays with Pseudomonas putida and Vibrio fischeri. Additional data on the toxicity to environmental bacteria were compiled from literature in order to assess the individual and expected joint bacterial toxicity of the pharmaceuticals in the mixture. The reported effluent concentration of the mixture was 15.4 nmol/l and the lowest experimentally obtained effect concentrations (EC10) were 242 nmol/l for microbial consortia in STPs, 225 nmol/l for P. putida and 73 nmol/l for V. fischeri. The lowest published effect concentrations (EC50) of the individual antibiotics in the mixture range between 15 and 150 nmol/l, whereas 0.9–190 μmol/l was the range of bacterial EC50 values found for the non-antibiotic mixture components. Pharmaceutical cocktails could shape microbial communities at concentrations relevant to STPs and the effluent receiving aquatic environment. The risk of antimicrobial mixture effects was completely dominated by the presence of antibiotics, whereas other pharmaceutical classes contributed only negligibly to the mixture toxicity. The joint bacterial toxicity can be accurately predicted from the individual toxicity of the mixture components, provided that standardized data on representative bacterial strains becomes available for all relevant compounds. These findings argue for a more sophisticated bacterial toxicity assessment of environmentally relevant pharmaceuticals, especially for those with a mode of action that is known to specifically affect prokaryotic microorganisms.
Afficher plus [+] Moins [-]Uptake and subcellular distribution of triclosan in typical hydrophytes under hydroponic conditions
2017
He, Yupeng | Nie, Enguang | Li, Chengming | Ye, Qingfu | Wang, Haiyan
The increasing discharge of pharmaceuticals and personal care products (PPCPs) into the environment has generated serious public concern. The recent awareness of the environmental impact of this emerging class of pollutants and their potential adverse effects on human health have been documented in many reports. However, information regarding uptake and intracellular distribution of PPCPs in hydrophytes under hydroponic conditions, and potential human exposure is very limited. A laboratory experiment was conducted using ¹⁴C-labeled triclosan (TCS) to investigate uptake and distribution of TCS in six aquatic plants (water spinach, purple perilla, cress, penny grass, cane shoot, and rice), and the subcellular distribution of ¹⁴C-TCS was determined in these plants. The results showed that the uptake and removal rate of TCS from nutrient solution by hydrophytes followed the order of cress (96%) > water spinach (94%) > penny grass (87%) > cane shoot (84%) > purple perilla (78%) > rice (63%) at the end of incubation period (192 h). The range of ¹⁴C-TCS content in the roots was 94.3%–99.0% of the added ¹⁴C-TCS, and the concentrations in roots were 2–3 orders of magnitude greater than those in shoots. Furthermore, the subcellular fraction-concentration factor (3.6 × 10²–2.6 × 10³ mL g⁻¹), concentration (0.58–4.47 μg g⁻¹), and percentage (30%–61%) of ¹⁴C-TCS in organelles were found predominantly greater than those in cell walls and/or cytoplasm. These results indicate that for these plants, the roots are the primary storage for TCS, and within plant cells organelles are the major domains for TCS accumulation. These findings provide a better understanding of translocation and accumulation of TCS in aquatic plants at the cellular level, which is valuable for environmental and human health assessments of TCS.
Afficher plus [+] Moins [-]Database-driven screening of South African surface water and the targeted detection of pharmaceuticals using liquid chromatography - High resolution mass spectrometry
2017
Wood, Timothy Paul | Du Preez, Christiaan | Steenkamp, Adriaan | Duvenage, Cornelia | Rohwer, Egmont R.
Pharmaceuticals and personal care products are released into aquatic environments, largely as a result of ineffectual removal during wastewater treatment. Here we present a screening strategy based on the use of three commercially available mass spectral databases, combined into a single searchable entity and parallelized by cluster computing. In addition to this, a targeted solid phase extraction method with Ultra High Pressure Liquid Chromatography coupled to quadrupole time of flight mass spectrometry (UHPLC-QTOF) was used to quantify 99 pharmaceuticals in South African surface water on a national level. Limits of quantification were in the low ng/L range for the majority of the compounds and it was found that nationally both Lamotrigine and Nevirapine occurred most often. Prednisolone and Ritonavir were present at the highest average concentration; 623 and 489 ng/L respectively. It is however shown that more than 50% of the targets chosen for analysis are not detectable in any of the samples, which highlights the utility of untargeted, database driven screening; prior to the use of costly analytical standards. Untargeted screening detected 45% of the compounds detected in targeted mode, and furthermore tentatively identified a total of 4273 unique compounds across the samples. Automatically triggered MS/MS analyses yielded 92 unique hits with greater than 95% confidence. It is therefore suggested that untargeted screening should precede the targeted approach as a matter of economy and to guide the selection of targets for quantification. There is however great room for improvement in current commercial database search methodologies as a large bottleneck exists due to processing time.
Afficher plus [+] Moins [-]Effects of acetylacetone on the photoconversion of pharmaceuticals in natural and pure waters
2017
Zhang, Guoyang | Wu, Bingdang | Zhang, Shujuan
Acetylacetone (AcAc) has proven to be a potent photo-activator in the degradation of color compounds. The effects of AcAc on the photochemical conversion of five colorless pharmaceuticals were for the first time investigated in both pure and natural waters with the UV/H2O2 process as a reference. In most cases, AcAc played a similar role to H2O2. For example, AcAc accelerated the photodecomposition of carbamazepine, oxytetracycline, and tetracycline in pure water. Meanwhile, the toxicity of tetracyclines and carbamazepine were reduced to a similar extent to that in the UV/H2O2 process. However, AcAc worked in a way different from that of H2O2. Based on the degradation kinetics, solvent kinetic isotope effect, and the inhibiting effect of O2, the underlying mechanisms for the degradation of pharmaceuticals in the UV/AcAc process were believed mainly to be direct energy transfer from excited AcAc to pharmaceuticals rather than reactive oxygen species-mediated reactions. In natural waters, dissolved organic matter (DOM) played a crucial role in the photoconversion of pharmaceuticals. The role of H2O2 became negligible due to the scavenging effects of DOM and inorganic ions. Interestingly, in natural waters, AcAc first accelerated the photodecomposition of pharmaceuticals and then led to a dramatic reduction with the depletion of dissolved oxygen. Considering the natural occurrence of diketones, the results here point out a possible pathway in the fate and transport of pharmaceuticals in aquatic ecosystems.
Afficher plus [+] Moins [-]Molecular toxicity of triclosan and carbamazepine to green algae Chlorococcum sp.: A single cell view using synchrotron-based fourier transform infrared spectromicroscopy
2017
Xin, Xiaying | Huang, Guohe | Liu, Xia | An, Chunjiang | Yao, Yao | Weger, Harold | Zhang, Peng | Chen, Xiujuan
Although pharmaceuticals and personal care products have been used and introduced into the environment in large quantities, little information on potential ecological risks is currently available considering their effects on living organisms. We verified the feasibility of using synchrotron-based mid-infrared (SR-FTIR) spectromicroscopy to explore in vivo toxic effects on single living Chlorococcum sp. cells. The study provided important information to achieve a better understanding of the toxic mechanism of triclosan and carbamazepine on living algae Chlorococcum sp. Triclosan and carbamazepine had distinctive toxic effects on unicellular living algae. Most strikingly, triclosan had more dramatic toxic effects on biochemical components than carbamazepine. Triclosan can affect algae primarily by inhibiting fatty acid synthesis and causing protein aggregation. The toxicity response was irreversible at higher concentrations (100.000 μM), but attenuated at lower concentrations (0.391 μM) as time passes. Carbamazepine can produce hydrophobic interactions to affect the phospholipid bilayer and work on specific proteins to disfunction the cell membrane. Carbamazepine-exposed cells developed a resistance while extending exposure time. This is the first demonstration from an ecological standpoint that SR-FTIR can provide an innovative approach to reveal the toxicity of emerging pollutants in aquatic environments.
Afficher plus [+] Moins [-]Determining potential adverse effects in marine fish exposed to pharmaceuticals and personal care products with the fish plasma model and whole-body tissue concentrations
2017
Meador, James P. | Yeh, Andrew | Gallagher, Evan P.
The Fish Plasma Model (FPM) was applied to water exposure and tissue concentrations in fish collected from two wastewater treatment plant impacted estuarine sites. In this study we compared predicted fish plasma concentrations to Cmax values for humans, which represents the maximum plasma concentration for the minimum therapeutic dose. The results of this study show that predictions of plasma concentrations for a variety of pharmaceutical and personal care products (PPCPs) from effluent concentrations resulted in 37 compounds (54%) exceeding the response ratio (RR = Fish [Plasma]/1%Cmaxtotal) of 1 compared to 3 compounds (14%) detected with values generated with estuarine receiving water concentrations. When plasma concentrations were modeled from observed whole-body tissue residues, 16 compounds out of 24 detected for Chinook (67%) and 7 of 14 (50%) for sculpin resulted in an RRtissue value greater than 1, which highlights the importance of this dose metric over that using estuarine water. Because the tissue residue approach resulted in a high percentage of compounds with calculated response ratios exceeding a value of unity, we believe this is a more accurate representation for exposure in the field. Predicting plasma concentrations from tissue residues improves our ability to assess the potential for adverse effects in fish because exposure from all sources is captured. Tissue residues are also more likely to represent steady-state conditions compared to those from water exposure because of the inherent reduction in variability usually observed for field data and the time course for bioaccumulation. We also examined the RR in a toxic unit approach to highlight the importance of considering multiple compounds exhibiting a similar mechanism of action.
Afficher plus [+] Moins [-]Degradation of Pharmaceuticals and Personal Care Products by White-Rot Fungi—a Critical Review
2017
Asif, Muhammad B. | Hai, Faisal I. | Singh, Lakhveer | Price, William E. | Nghiem, Long D.
White-rot fungi (WRF) mediated treatment can offer an environmentally friendly platform for the removal of pharmaceuticals and personal care products (PPCPs) from wastewater. These PPCPs may have adverse impacts on aquatic organisms and even human and thus their removal during wastewater treatment is of significant interest to the water industry. Whole-cell WRF or their extracellular lignin modifying enzymes (LMEs) have been reported to efficiently degrade PPCPs that are persistent to conventional activated sludge process. WRF mediated treatment of PPCPs depends on a number of factors including physicochemical properties of PPCPs (e.g., hydrophobicity and chemical structure) and wastewater matrix (e.g., pH, temperature, and dissolved constituents), type of WRF species and their specific extracellular enzymes. This review critically analyzes the performance of whole-cell WRF and their LMEs for the removal of PPCPs; particularly, it offers insights into PPCP removal mechanisms (e.g., biosorption vs. biodegradation) and degradation pathways as well as the formation of intermediate byproducts.
Afficher plus [+] Moins [-]Photodegradation of diclofenac in seawater by simulated sunlight irradiation: The comprehensive effect of nitrate, Fe(III) and chloride
2017
Zhang, N. | Li, J.M. | Liu, G.G. | Chen, X.L. | Jiang, K.
Diclofenac is one of the most frequently detected pharmaceuticals in various aquatic environments. The photodegradation of diclofenac in the absence/presence of nitrate, Fe(III) and chloride, especially their interactions, were systematically studied. Under the study conditions, photodegradation rate was decreased with increasing nitrate, Fe(III) and chloride concentrations. Nitrate has an synergistic action for Fe(III). Nitrate and chloride have antagonistic effect. An antagonistic action is present between nitrate, Fe(III) and chloride. Moreover, a simple linear model which very well describes the results is given.
Afficher plus [+] Moins [-]Occurrence of pharmaceuticals and UV-filters in riverine run-offs and waters of the German Baltic Sea
2017
Fisch, Kathrin | Waniek, J. J. (Joanna J.) | Schulz-Bull, Detlef E.
The occurrence of pharmaceuticals and personal care products (PPCPs) in the marine environment is of great concern. This study was done to determine the emergence of eight pharmaceuticals and eleven ultraviolet filters (UV-Filters) in 5 rivers/streams discharging into the Baltic Sea. Furthermore, a focus was put on the influence of wastewater treatment plant as indirect source and the occurrence of the PPCPs in close beach proximity. Two pharmaceuticals (sulfamethoxazole, salicylic acid) and two UV-filters (2-phenylbenzimidazole-5-sulfonic acid, octocrylene) were detected in all analyzed water samples, with concentration ranging from 0.6ng/L to 836.3ng/L. In all rivers the PPCP concentration decreases towards the Baltic Sea. Sulfamethoxazole was detected at comparable concentration along the coast, which leads to the assumption of stable concentration in beach proximity. Along the coast UV-filters appeared in varying concentrations, leading to the conclusion that the direct input into the marine environment plays a bigger role than the indirect input.
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