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Total Oxidizable Precursors Assay for PFAS in Human Serum

Cioni, Lara; Nikiforov, Vladimir; Miranda Fernandes Coelho, Ana Carolina; Sandanger, Torkjel M; Herzke, Dorte

Per- and polyfluoroalkyl substances (PFAS) are a class of chemicals including over 4700 substances. As a limited number of PFAS is routinely analyzed in human serum, complementary analytical methods are required to characterize the overlooked fraction. A promising tool is the total oxidizable precursors (TOP) assay to look for precursors by oxidation to perfluoroalkyl acids (PFAA). The TOP assay was originally developed for large volumes of water and had to be adapted for 250 μL of human serum. Optimization of the method was performed on serum samples spiked with model precursors. Oxidative conditions similar to previous TOP assay methods were not sufficient for complete oxidation of model precursors. Prolonged heating time (24 h) and higher oxidant amount (95 mg of Na2S2O8 per 225 μL of serum) were needed for complete conversion of the model precursors and accomplishing PFAA yields of 35–100 %. As some precursors are not fully converted to PFAA, the TOP assay can only provide semi-quantitative estimates of oxidizable precursors in human serum. However, the TOP assay can be used to give indications about the identity of unknown precursors by evaluating the oxidation products, including perfluoroalkyl sulfonic acids (PFSA) and perfluoroalkyl ether carboxylic acids (PFECA). The optimized TOP assay for human serum opens the possibility for high-throughput screening of human serum for undetected PFAA precursors.

Elsevier

2022

Targeted PFAS analyses and Extractable Organofluorine – Enhancing our Understanding of the presence of unknown PFAS in Norwegian wildlife

Herzke, Dorte; Nikiforov, Vladimir; Yeung, Leo WY.; Moe, Børge; Routti, Heli Anna Irmeli; Nygård, Torgeir; Gabrielsen, Geir W.; Hanssen, Linda

With the current possible presence of thousands of PFAS compounds in industrial emissions, there is an increasing need to assess the impacts of PFAS regulation of conventional PFAS on one hand and the exposure to emerging and yet unknown PFAS on the other. Today’s analytical methodologies using targeted approaches are not sufficient to determine the complete suite of PFAS present. To evaluate the presence of unknown PFAS, we investigated in this study the occurrence of an extended range of target PFAS in various species from the marine and terrestrial Norwegian environment, in relation to the extractable organic fluorine (EOF), which yields the total amount of organic fluorine. The results showed a varying presence of extractable fluorinated organics, with glaucous gull eggs, otter liver and polar bear plasma showing the highest EOF and a high abundance of PFAS as well. The targeted PFAS measurements explained 1% of the organic fluorine for moose liver as the lowest and 94% for otter liver as the highest. PFCAs like trifluoro acetic acid (TFA, reported semi-quantitatively), played a major role in explaining the organic fluorine present. Emerging PFAS as the perfluoroethylcyclohexane sulfonate (PFECHS), was found in polar bear plasma in quantifiable amounts for the first time, confirming earlier detection in arctic species far removed from emission sources. To enable a complete organic fluorine mass balance in wildlife, new approaches are needed, to uncover the presence of new emerging PFAS as cyclic- or ether PFAS together with chlorinated PFAS as well as fluorinated organic pesticides and pharmaceuticals.

Elsevier

2022

An In Vitro Dosimetry Tool for the Numerical Transport Modeling of Engineered Nanomaterials Powered by the Enalos RiskGONE Cloud Platform

Cheimarios, Nikolaos; Pem, Barbara; Tsoumanis, Andreas; Ilic, Krunoslav; Vrček, Ivana Vinković; Melagraki, Georgia; Bitounis, Dimitrios; Isigonis, Panagiotis; Dusinska, Maria; Lynch, Iseult; Demokritou, Philip; Afantitis, Antreas

A freely available “in vitro dosimetry” web application is presented enabling users to predict the concentration of nanomaterials reaching the cell surface, and therefore available for attachment and internalization, from initial dispersion concentrations. The web application is based on the distorted grid (DG) model for the dispersion of engineered nanoparticles (NPs) in culture medium used for in vitro cellular experiments, in accordance with previously published protocols for cellular dosimetry determination. A series of in vitro experiments for six different NPs, with Ag and Au cores, are performed to demonstrate the convenience of the web application for calculation of exposure concentrations of NPs. Our results show that the exposure concentrations at the cell surface can be more than 30 times higher compared to the nominal or dispersed concentrations, depending on the NPs’ properties and their behavior in the cell culture medium. Therefore, the importance of calculating the exposure concentration at the bottom of the cell culture wells used for in vitro arrays, i.e., the particle concentration at the cell surface, is clearly presented, and the tool introduced here allows users easy access to such calculations. Widespread application of this web tool will increase the reliability of subsequent toxicity data, allowing improved correlation of the real exposure concentration with the observed toxicity, enabling the hazard potentials of different NPs to be compared on a more robust basis.

MDPI

2022

An NO2 sensor based on WO3 thin films for automotive applications in the microwave frequency range

Paleczek, Anna; Grochala, D.; Staszek, K.; Gruszczynski, S.; Maciak, Erwin; Opilski, Zbigniew; Kaluzynski, Piotr; Wojcikowski, Marek; Cao, Tuan-Vu; Rydosz, A.

2022

Plastic burdens in northern fulmars from Svalbard: looking back 25 years

Collard, France; Bangjord, Georg; Herzke, Dorte; Gabrielsen, Geir Wing

The northern fulmar Fulmarus glacialis ingests a larger number of (micro)plastics than many other seabirds due to its feeding habits and gut morphology. Since 2002, they are bioindicators of marine plastics in the North Sea region, and data are needed to extend the programme to other parts of their distribution areas, such as the Arctic. In this study, we provide data on ingested plastics by fulmars collected in 1997 in Kongsfjorden, Svalbard. An extraction protocol with KOH was used and for half of the birds, the gizzard and the proventricular contents were analysed separately. Ninety-one percent of the birds had ingested at least one piece of plastic with an average of 10.3 (±11.9 SD) pieces. The gizzards contained significantly more plastics than the proventriculus. Hard fragments and polyethylene were the most common characteristics. Twelve percent of the birds exceeded the EcoQO value of 0.1 g.

Elsevier

2022

Plastic ingestion and associated additives in Faroe Islands chicks of the Northern Fulmar Fulmarus glacialis

Collard, France; Leconte, Simon; Danielsen, Johannis; Halsband, Claudia; Herzke, Dorte; Harju, Mikael; Tulatz, Felix; Gabrielsen, Geir Wing; Tarroux, Arnaud

Northern Fulmars (Fulmarus glacialis) are a pelagic seabird species distributed at northern and polar latitudes. They are often used as an indicator of plastic pollution in the North Sea region, but data are lacking from higher latitudes, especially when it comes to chicks. Here, we investigated amounts of ingested plastic and their characteristics in fulmar chicks from the Faroe Islands. Plastic particles (1 mm) in chicks of two age classes were searched using a digestion method with KOH. In addition, to evaluate if additive tissue burden reflects plastic ingestion, we measured liver tissue concentrations of two pollutant classes associated with plastic materials: polybrominated diphenyl ethers (PBDEs) and several dechloranes, using gas chromatography with high-resolution mass spectrometry. The most common shape was hard fragment (81%) and the most common polymer was polyethylene (73%). Plastic contamination did not differ between either age class, and we found no correlation between neither the amount and mass of plastic particles and the concentration of additives. After comparison with previous studies on adult fulmars, we do not recommend using chicks for biomonitoring adults because chicks seem to ingest more plastics than adults.

2022

Plastics as a carrier of chemical additives to the Arctic: possibilities for strategic monitoring across the circumpolar North

Hamilton, Bonnie M.; Baak, Julia E.; Vorkamp, Katrin; Hammer, Sjúrður; Granberg, Maria; Herzke, Dorte; Provencher, Jennifer F.

Plastic pollution (including microplastics) has been reported in a variety of biotic and abiotic compartments across the circumpolar Arctic. Due to their environmental ubiquity, there is a need to understand not only the fate and transport of physical plastic particles, but also the fate and transport of additive chemicals associated with plastic pollution. Further, there is a fundamental research gap in understanding long-range transport of chemical additives to the Arctic via plastics as well as their behavior under environmentally relevant Arctic conditions. Here, we comment on the state of the science of plastic as carriers of chemical additives to the Arctic, and highlight research priorities going forward. We suggest further research on the transport pathways of chemical additives via plastics from both distant and local sources and laboratory experiments to investigate chemical behavior of plastic additives under Arctic conditions, including leaching, uptake, and bioaccumulation. Ultimately, chemical additives need to be included in strategic monitoring efforts to fully understand the contaminant burden of plastic pollution in Arctic ecosystems.

2022

Comparison of particle number size distribution trends in ground measurements and climate models

Leinonen, Ville; Kokkola, Harri; Yli-Juuti, Taina; Mielonen, Tero; Kühn, Thomas; Nieminen, Tuomo; Heikkinen, Simo; Miinalainen, Tuuli; Bergman, Tommi; Carslaw, Ken; Decesari, Stefano; Fiebig, Markus; Hussein, Tareq; Kivekäs, Niku; Krejci, Radovan; Kulmala, Markku; Leskinen, Ari; Massling, Andreas; Mihalopoulos, Nikos; Mulcahy, Jane P.; Noe, Steffen M.; Van Noije, Twan; O'connor, Fiona M.; O'dowd, Colin; Oliviè, Dirk Jan Leo; Pernov, Jakob B.; Petäjä, Tuukka; Seland, Øyvind; Schulz, Michael; Scott, Catherine E.; Skov, Henrik; Swietlicki, Erik; Tuch, Thomas; Wiedensohler, Alfred; Virtanen, Annele; Mikkonen, Santtu

Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.

2022

An actionable annotation scoring framework for gas chromatography-high-resolution mass spectrometry

Koelmel, Jeremy P.; Xie, Hongyu; Price, Elliott J.; Lin, Elizabeth; Manz, Katherine E.; Stelben, Paul J.; Paige, Matthew K.; Papazian, Stefano; Okeme, Joseph; Rostkowski, Pawel Marian; Nikiforov, Vladimir; Wang, Thanh; Hu, Xin; Lai, Yunjia; Miller, Gary W.; Walker, Douglas; Martin, Jonathan W.; Pollitt, Krystal J. Godri

Omics-based technologies have enabled comprehensive characterization of our exposure to environmental chemicals (chemical exposome) as well as assessment of the corresponding biological responses at the molecular level (eg, metabolome, lipidome, proteome, and genome). By systematically measuring personal exposures and linking these stimuli to biological perturbations, researchers can determine specific chemical exposures of concern, identify mechanisms and biomarkers of toxicity, and design interventions to reduce exposures. However, further advancement of metabolomics and exposomics approaches is limited by a lack of standardization and approaches for assigning confidence to chemical annotations. While a wealth of chemical data is generated by gas chromatography high-resolution mass spectrometry (GC-HRMS), incorporating GC-HRMS data into an annotation framework and communicating confidence in these assignments is challenging. It is essential to be able to compare chemical data for exposomics studies across platforms to build upon prior knowledge and advance the technology. Here, we discuss the major pieces of evidence provided by common GC-HRMS workflows, including retention time and retention index, electron ionization, positive chemical ionization, electron capture negative ionization, and atmospheric pressure chemical ionization spectral matching, molecular ion, accurate mass, isotopic patterns, database occurrence, and occurrence in blanks. We then provide a qualitative framework for incorporating these various lines of evidence for communicating confidence in GC-HRMS data by adapting the Schymanski scoring schema developed for reporting confidence levels by liquid chromatography HRMS (LC-HRMS). Validation of our framework is presented using standards spiked in plasma, and confident annotations in outdoor and indoor air samples, showing a false-positive rate of 12% for suspect screening for chemical identifications assigned as Level 2 (when structurally similar isomers are not considered false positives). This framework is easily adaptable to various workflows and provides a concise means to communicate confidence in annotations. Further validation, refinements, and adoption of this framework will ideally lead to harmonization across the field, helping to improve the quality and interpretability of compound annotations obtained in GC-HRMS.

2022

The miniaturized enzyme-modified comet assay for genotoxicity testing of nanomaterials

El Yamani, Naouale; Rundén-Pran, Elise; Collins, Andrew Richard; Longhin, Eleonora Marta; Elje, Elisabeth; Hoet, Peter; Vrček, Ivana Vinković; Doak, Shareen H.; Fessard, Valérie; Dusinska, Maria

The in vitro comet assay is a widely applied method for investigating genotoxicity of chemicals including engineered nanomaterials (NMs). A big challenge in hazard assessment of NMs is possible interference between the NMs and reagents or read-out of the test assay, leading to a risk of biased results. Here, we describe both the standard alkaline version of the in vitro comet assay with 12 mini-gels per slide for detection of DNA strand breaks and the enzyme-modified version that allows detection of oxidized DNA bases by applying lesion-specific endonucleases (e.g., formamidopyrimidine DNA glycosylase or endonuclease III). We highlight critical points that need to be taken into consideration when assessing the genotoxicity of NMs, as well as basic methodological considerations, such as the importance of carrying out physicochemical characterization of the NMs and investigating uptake and cytotoxicity. Also, experimental design—including treatment conditions, cell number, cell culture, format and volume of medium on the plate—is crucial and can have an impact on the results, especially when testing NMs. Toxicity of NMs depends upon physicochemical properties that change depending on the environment. To facilitate testing of numerous NMs with distinct modifications, the higher throughput miniaturized version of the comet assay is essential.

Frontiers Media S.A.

2022

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