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Can plastic related chemicals be indicators of plastic ingestion in an Arctic seabird?

Collard, France; Tulatz, Felix; Harju, Mikael; Herzke, Dorte; Bourgeon, Sophie; Gabrielsen, Geir Wing

For decades, the northern fulmar (Fulmarus glacialis) has been found to ingest and accumulate high loads of plastic due to its feeding ecology and digestive tract morphology. Plastic ingestion can lead to both physical and toxicological effects as ingested plastics can be a pathway for hazardous chemicals into seabirds' tissues. Many of these contaminants are ubiquitous in the environment and the contribution of plastic ingestion to the uptake of those contaminants in seabirds’ tissues is poorly known. In this study we aimed at quantifying several plastic-related chemicals (PRCs) -PBDE209, several dechloranes and several phthalate metabolites- and assessing their relationship with plastic burdens (both mass and number) to further investigate their potential use as proxies for plastic ingestion. Blood samples from fulmar fledglings and liver samples from both fledgling and non-fledgling fulmars were collected for PRC quantification. PBDE209 and dechloranes were quantified in 39 and 33 livers, respectively while phthalates were quantified in plasma. Plastic ingestion in these birds has been investigated previously and showed a higher prevalence in fledglings. PBDE209 was detected in 28.2 % of the liver samples. Dechlorane 602 was detected in all samples while Dechloranes 601 and 604 were not detected in any sample. Dechlorane 603 was detected in 11 individuals (33%). Phthalates were detected in one third of the analysed blood samples. Overall, no significant positive correlation was found between plastic burdens and PRC concentrations. However, a significant positive relationship between PBDE209 and plastic number was found in fledglings, although likely driven by one outlier. Our study shows the complexity of PRC exposure, the timeline of plastic ingestion and subsequent uptake of PRCs into the tissues in birds, the additional exposure of these chemicals via their prey, even in a species ingesting high loads of plastic.

Elsevier

2024

Air pollution emission inventory using national high-resolution spatial parameters for the Nordic countries and analysis of PM2.5 spatial distribution for road transport and machinery and off-road sectors

Paunu, Ville-Veikko; Karvosenoja, Niko; Segersson, David; Lopez-Aparicio, Susana; Nielsen, Ole-Kenneth; Plejdrup, Marlene S.; Thorsteinsson, Throstur; Vo, Dam Thanh; Kuenen, Jeroen; van der Gon, Hugo Denier; Jalkanen, Jukka-Pekka; Brandt, Jørgen; Geels, Camilla

Air pollution is an important cause of adverse health effects, even in the Nordic countries, which have relatively good air quality. Modelling-based air quality assessment of the health impacts relies on reliable model estimates of ambient air pollution concentrations, which furthermore rely on good-quality spatially resolved emission data. While quantitative emission estimates are the cornerstone of good emission data, description of the spatial distribution of the emissions is especially important for local air quality modelling at high resolution. In this paper we present a new air pollution emission inventory for the Nordic countries with high-resolution spatial allocation (1 km × 1 km) covering the years 1990, 1995, 2000, 2005, 2010, 2012, and 2014. The inventory is available at https://doi.org/10.5281/zenodo.10571094 (Paunu et al., 2023). To study the impact of applying national data and methods to the spatial distribution of the emissions, we compared road transport and machinery and off-road sectors to CAMS-REGv4.2, which used a consistent spatial distribution method throughout Europe for each sector. Road transport is a sector with well-established proxies for spatial distribution, while for the machinery and off-road sector, the choice of proxies is not as straightforward as it includes a variety of different type of vehicles and machines operating in various environments. We found that CAMS-REGv4.2 was able to produce similar spatial patterns to our Nordic inventory for the selected sectors. However, the resolution of our Nordic inventory allows for more detailed impact assessment than CAMS-REGv4.2, which had a resolution of 0.1° × 0.05° (longitude–latitude, roughly 5.5 km × 3.5–6.5 km in the Nordic countries). The EMEP/EEA Guidebook chapter on spatial mapping of emissions has recommendations for the sectoral proxies. Based on our analysis we argue that the guidebook should have separate recommendations for proxies for several sub-categories of the machinery and off-road sectors, instead of including them within broader sectors. We suggest that land use data are the best starting point for proxies for many of the subsectors, and they can be combined with other suitable data to enhance the spatial distribution. For road transport, measured traffic flow data should be utilized where possible, to support modelled data in the proxies.

2024

New insights from an eight-year study on per- and polyfluoroalkyl substances in an urban terrestrial ecosystem

Heimstad, Eldbjørg Sofie; Nygård, Torgeir; Moe, Børge; Herzke, Dorte

Per- and polyfluoroalkyl substances (PFAS) were analysed in a high number of terrestrial samples of soil, earthworm, bird eggs and liver from red fox and brown rat in an urban area in Norway from 2013 to 2020. PFOS and the long chain PFCAs were the most dominating compounds in all samples, proving their ubiquitous distribution. Other less studied compounds such as 6:2 FTS were first and foremost detected in earthworm. 8:2 FTS was found in many samples of fieldfare egg, sparrowhawk egg and earthworm, where the eggs had highest concentrations. Highest concentrations for both 6:2 FTS and 8:2 FTS were detected at present and former industry areas. FOSA was detected in many samples of the species with highest concentrations in red fox liver and brown rat liver of 3.3 and 5.5 ng/g ww.

PFAS concentrations from the urban area were significantly higher than from background areas indicating that some of the species can be suitable as markers for PFAS emissions in an urban environment. Fieldfare eggs had surprisingly high concentrations of PFOS and PFCA concentrations from areas known to be or have been influenced by industry. Biota-soil-accumulation factor and magnification calculations indicate accumulation and magnification potential for several PFAS.

Earthworm and fieldfare egg had average concentrations above the Canadian and European thresholds in diet for avian wildlife and predators. For earthworms, 18 % of the samples exceeded the European threshold (33 ng/g ww) of PFOS in prey for predators, and for fieldfare eggs, 35 % of the samples were above the same threshold. None of the soil samples exceeded a proposed PNEC of PFOS for soil living organisms of 373 ng/g dw.

Elsevier

2024

Widespread Pesticide Distribution in the European Atmosphere Questions their Degradability in Air

Mayer, Ludovic; Degrendele, Celine; Senk, Petr; Kohoutek, Jiří; Přibylovác, Petra; Kukučka, Petr; Melymuk, Lisa; Durand, Amandine; Ravier, Sylvain; Alastuey, Andres; Baker, Alex R.; Baltensperger, Urs; Baumann-Stanzer, Kathrin; Biermann, Tobias; Bohlin-Nizzetto, Pernilla; Ceburnis, Darius; Conil, Sébastien; Couret, Cedric; Degorska, Anna; Diapouli, Evangelia; Eckhardt, Sabine; Eleftheriadis, Konstantinos; Forster, Grant L.; Freier, Korbinian; Gheusi, Francois; Gini, Maria; Hellén, Heidi; Henne, Stephan; Hermann, Hartmut; Šmejkalová, Adéla Holubová; Horrak, Urmas; Hüglin, Christoph; Junninen, Heikki; Kristensson, Adam; Langrene, Laurent; Levula, Janne; Lothon, Marie; Ludewig, Elke; Makkonen, Ulla; Matejovičová, Jana; Mihalopoulos, Nikolaos; Mináriková, Veronika; Moche, Wolfgang; Noe, Steffen M.; Perez, Noemi; Petäjä, Tuukka; Pont, Veronique; Poulain, Laurent; Quivet, Etienne; Ratz, Gabriela; Rehm, Till; Reimann, Stefan; Simmons, Ivan; Sonke, Jeroen E.; Sorribas, Mar; Spoor, Ronald; Swart, Daan P.J.; Vasilatou, Vasiliki; Wortham, Henri; Yela, Margarita; Zarmpas, Pavlos; Zellweger-Fäsi, Claudia; Tørseth, Kjetil; Laj, Paolo G.; Klanova, Jana; Lammel, Gerhard

Risk assessment of pesticide impacts on remote ecosystems makes use of model-estimated degradation in air. Recent studies suggest these degradation rates to be overestimated, questioning current pesticide regulation. Here, we investigated the concentrations of 76 pesticides in Europe at 29 rural, coastal, mountain, and polar sites during the agricultural application season. Overall, 58 pesticides were observed in the European atmosphere. Low spatial variation of 7 pesticides suggests continental-scale atmospheric dispersal. Based on concentrations in free tropospheric air and at Arctic sites, 22 pesticides were identified to be prone to long-range atmospheric transport, which included 15 substances approved for agricultural use in Europe and 7 banned ones. Comparison between concentrations at remote sites and those found at pesticide source areas suggests long atmospheric lifetimes of atrazine, cyprodinil, spiroxamine, tebuconazole, terbuthylazine, and thiacloprid. In general, our findings suggest that atmospheric transport and persistence of pesticides have been underestimated and that their risk assessment needs to be improved.

2024

Composition and sources of carbonaceous aerosol in the European Arctic at Zeppelin Observatory, Svalbard (2017 to 2020)

Yttri, Karl Espen; Bäcklund, Are; Conen, Franz; Eckhardt, Sabine; Evangeliou, Nikolaos; Fiebig, Markus; Kasper-Giebl, Anne; Gold, Avram; Gundersen, Hans; Myhre, Cathrine Lund; Platt, Stephen Matthew; Simpson, David; Surratt, Jason D.; Szidat, Sönke; Rauber, Martin; Tørseth, Kjetil; Ytre-Eide, Martin Album; Zhang, Zhenfa; Aas, Wenche

We analyzed long-term measurements of organic carbon, elemental carbon, and source-specific organic tracers from 2017 to 2020 to constrain carbonaceous aerosol sources in the rapidly changing Arctic. Additionally, we used absorption photometer (Aethalometer) measurements to constrain equivalent black carbon (eBC) from biomass burning and fossil fuel combustion, using positive matrix factorization (PMF).

Our analysis shows that organic tracers are essential for understanding Arctic carbonaceous aerosol sources. Throughout 2017 to 2020, levoglucosan exhibited bimodal seasonality, reflecting emissions from residential wood combustion (RWC) in the heating season (November to May) and from wildfires (WFs) in the non-heating season (June to October), demonstrating a pronounced interannual variability in the influence of WF. Biogenic secondary organic aerosol (BSOA) species (2-methyltetrols) from isoprene oxidation was only present in the non-heating season, peaking in July to August. Warm air masses from Siberia led to a substantial increase in 2-methyltetrols in 2019 and 2020 compared to 2017 to 2018. This highlights the need to investigate the contribution of local sources vs. long-range atmospheric transport (LRT), considering the temperature sensitivity of biogenic volatile organic compound emissions from Arctic vegetation. Tracers of primary biological aerosol particles (PBAPs), including various sugars and sugar alcohols, showed elevated levels in the non-heating season, although with different seasonal trends, whereas cellulose had no apparent seasonality. Most PBAP tracers and 2-methyltetrols peaked during influence of WF emissions, highlighting the importance of measuring a range of source-specific tracers to understand sources and dynamics of carbonaceous aerosol. The seasonality of carbonaceous aerosol was strongly influenced by LRT episodes, as background levels are extremely low. In the non-heating season, the organic aerosol peak was as influenced by LRT, as was elemental carbon during the Arctic haze period.

Source apportionment of carbonaceous aerosol by Latin hypercube sampling showed mixed contributions from RWC (46 %), fossil fuel (FF) sources (27 %), and BSOA (25 %) in the heating season. In contrast, the non-heating season was dominated by BSOA (56 %), with lower contributions from WF (26 %) and FF sources (15 %).

Source apportionment of eBC by PMF showed that FF combustion dominated eBC (70±2.7 %), whereas RWC (22±2.7 %) was more abundant than WF (8.0±2.9 %). Modeled BC concentrations from FLEXPART (FLEXible PARTicle dispersion model) attributed an almost equal share to FF sources (51±3.1 %) and to biomass burning. Both FLEXPART and the PMF analysis concluded that RWC is a more important source of (e)BC than WF. However, with a modeled RWC contribution of 30±4.1 % and WF of 19±2.8 %, FLEXPART suggests relatively higher contributions to eBC from these sources. Notably, the BB fraction of EC was twice as high as that of eBC, reflecting methodological differences between source apportionment by LHS and PMF. However, important conclusions drawn are unaffected, as both methods indicate the presence of RWC- and WF-sourced BC at Zeppelin, with a higher relative BB contribution during the non-heating season.

In summary, organic aerosol (281±106 ng m−3) constitutes a significant fraction of Arctic PM10, although surpassed by sea salt aerosol (682±46.9 ng m−3), mineral dust (613±368 ng m−3), and typically non-sea-salt sulfate SO (314±62.6 ng m−3), originating mainly from anthropogenic sources in winter and from natural sources in summer.

2024

Recommendations for reporting equivalent black carbon (eBC) mass concentrations based on long-term pan-European in-situ observations

Savadkoohi, Marjan; Pandolfi, Marco; Favez, Olivier; Putaud, Jean-Philippe; Eleftheriadis, Konstantinos; Fiebig, Markus; Hopke, Philip K.; Laj, Paolo G.; Wiedensohler, Alfred; Alados-Arboledas, Lucas; Bastian, Susanne; Chazeau, Benjamin; Maria, Alvaro Clemente; Colombi, Cristina; Costabile, Francesca; Green, David C.; Hueglin, Christoph; Liakakou, Eleni; Luoma, Krista; Listrani, Stefano; Mihalopoulos, Nikos; Marchand, Nicolas; Močnik, Griša; Niemi, Jarkko V; Ondráček, Jakub; Petit, Jean Eudes; Rattigan, Oliver V.; Reche, Cristina; Timonen, Hilkka; Titos, Gloria; Tremper, Anja H.; Vratolis, Stergios; Vodicka, Petr; Funes, Eduardo Yubero; Zíková, Naděžda; Harrison, Roy M.; Petäjä, Tuukka; Alastuey, Andrés; Querol, Xavier

A reliable determination of equivalent black carbon (eBC) mass concentrations derived from filter absorption photometers (FAPs) measurements depends on the appropriate quantification of the mass absorption cross-section (MAC) for converting the absorption coefficient (babs) to eBC. This study investigates the spatial–temporal variability of the MAC obtained from simultaneous elemental carbon (EC) and babs measurements performed at 22 sites. We compared different methodologies for retrieving eBC integrating different options for calculating MAC including: locally derived, median value calculated from 22 sites, and site-specific rolling MAC. The eBC concentrations that underwent correction using these methods were identified as LeBC (local MAC), MeBC (median MAC), and ReBC (Rolling MAC) respectively. Pronounced differences (up to more than 50 %) were observed between eBC as directly provided by FAPs (NeBC; Nominal instrumental MAC) and ReBC due to the differences observed between the experimental and nominal MAC values. The median MAC was 7.8 ± 3.4 m2 g-1 from 12 aethalometers at 880 nm, and 10.6 ± 4.7 m2 g-1 from 10 MAAPs at 637 nm. The experimental MAC showed significant site and seasonal dependencies, with heterogeneous patterns between summer and winter in different regions. In addition, long-term trend analysis revealed statistically significant (s.s.) decreasing trends in EC. Interestingly, we showed that the corresponding corrected eBC trends are not independent of the way eBC is calculated due to the variability of MAC. NeBC and EC decreasing trends were consistent at sites with no significant trend in experimental MAC. Conversely, where MAC showed s.s. trend, the NeBC and EC trends were not consistent while ReBC concentration followed the same pattern as EC. These results underscore the importance of accounting for MAC variations when deriving eBC measurements from FAPs and emphasize the necessity of incorporating EC observations to constrain the uncertainty associated with eBC.

Elsevier

2024

Hazard assessment of nanomaterials using in vitro toxicity assays: Guidance on potential assay interferences and mitigating actions to avoid biased results

El Yamani, Naouale; Rundén-Pran, Elise; Varet, Julia; Beus, Maja; Dusinska, Maria; Fessard, Valerie; Moschini, Elisa; Serchi, Tommaso; Cimpan, Mihaela Roxana; Lynch, Iseult; Vinković Vrček, ivana

The movement towards an animal-free testing approach for risk assessment represents a key paradigm shift in toxicology. Risk assessment of engineered and anthropogenic nanoscale materials (NM) is dependent on reliable hazard characterization, which requires validated test methods and models, and increasingly on mechanistic insights into the mode of action. The properties that make NMs so advantageous for a wide range of commercial and industrial applications also pose a challenge when it comes to safety testing under in vitro and in chemico experimental settings. Their large reactive surface area makes NMs prone to interactions with assay reagents, readout signals, or intermediate steps of many test assays, leading to the potential for biased results and data inconsistencies, collectively referred to as interferences. Therefore, methods and protocols developed and validated for conventional chemicals often require adaptation and checking for reliability in NMs' toxicity assessment. This review presents the collected scientific knowledge on NMs-induced interferences for the most common in vitro toxicity assays and methods related to cytotoxicity, oxidative stress and inflammatory response evaluation. Our analysis of existing scientific literature showed that the challenge of NMs-induced interference was not explicitly addressed in more than 90% of the papers published up to 2014 reporting the safety and toxicity of NMs. In later years, increasing number of studies tackled the interference challenge in toxicity testing of NMs, which initiated exhaustive work on standardization and validation of existing regulatory-relevant in vitro test protocols and guidelines. Due to the specificity of the different NMs and the range of ways they can potentially interfere with in vitro assays, interference and fit-for purpose controls should be included for each NM type and method applied, unless label-free assays are selected. Here, we provide a decision tree to guide researchers on how to design experiments to avoid interferences during in vitro testing by taking appropriate mitigation actions and how to include proper interference controls in their experimental design where complete avoidance is not possible. The application of this decision tree will improve the reliability, comparability and reusability of in vitro toxicity data on engineered NMs or ENMs, increasing the relevance of in silico hazard data for use in risk assessment and in science-based risk governance of NMs. The approach is applicable more broadly also, to advanced materials and to hazard assessment of anthropogenic nanoscale materials such as microplastic and tyre-wear particles.

Elsevier

2024

Aircraft-based mass balance estimate of methane emissions from offshore gas facilities in the southern North Sea

Pühl, Magdalena; Roiger, Anke; Fiehn, Alina; Gorchov Negron, Alan M.; Kort, Eric A.; Schwietzke, Stefan; Pisso, Ignacio; Foulds, Amy; Lee, James; France, James L.; Jones, Anna E.; Lowry, Dave; Fisher, Rebecca E.; Huang, Langwen; Shaw, Jacob; Bateson, Prudence; Andrews, Stephen; Young, Stuart; Dominutti, Pamela; Lachlan-Cope, Tom; Weiss, Alexandra; Allen, Grant

Atmospheric methane (CH4) concentrations have more than doubled since the beginning of the industrial age, making CH4 the second most important anthropogenic greenhouse gas after carbon dioxide (CO2). The oil and gas sector represents one of the major anthropogenic CH4 emitters as it is estimated to account for 22 % of global anthropogenic CH4 emissions. An airborne field campaign was conducted in April–May 2019 to study CH4 emissions from offshore gas facilities in the southern North Sea with the aim of deriving emission estimates using a top-down (measurement-led) approach. We present CH4 fluxes for six UK and five Dutch offshore platforms or platform complexes using the well-established mass balance flux method. We identify specific gas production emissions and emission processes (venting and fugitive or flaring and combustion) using observations of co-emitted ethane (C2H6) and CO2. We compare our top-down estimated fluxes with a ship-based top-down study in the Dutch sector and with bottom-up estimates from a globally gridded annual inventory, UK national annual point-source inventories, and operator-based reporting for individual Dutch facilities. In this study, we find that all the inventories, except for the operator-based facility-level reporting, underestimate measured emissions, with the largest discrepancy observed with the globally gridded inventory. Individual facility reporting, as available for Dutch sites for the specific survey date, shows better agreement with our measurement-based estimates. For all the sampled Dutch installations together, we find that our estimated flux of (122.9 ± 36.8) kg h−1 deviates by a factor of 0.64 (0.33–12) from reported values (192.8 kg h−1). Comparisons with aircraft observations in two other offshore regions (the Norwegian Sea and the Gulf of Mexico) show that measured, absolute facility-level emission rates agree with the general distribution found in other offshore basins despite different production types (oil, gas) and gas production rates, which vary by 2 orders of magnitude. Therefore, mitigation is warranted equally across geographies.

2024

Air-soil cycling of oxygenated, nitrated and parent polycyclic aromatic hydrocarbons in source and receptor areas

Mwangi, John K.; Degrendele, Celine; Bandowe, Benjamin A. M.; Bohlin-Nizzetto, Pernilla; Halse, Anne Karine; Šmejkalová, Adela Holubová; Kim, Jun-Tae; Kukučka, Petr; Martiník, Jakub; Nežiková, Barbora Palátová; Přibylová, Petra; Prokeš, Roman; Sáňka, Milan; Tannous, Mariam; Vinkler, Jakub; Lammel, Gerhard

Elsevier

2024

Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)

Thompson, Rona Louise; Montzka, Stephen A.; Vollmer, Martin K.; Arduini, Jgor; Crotwell, Molly; Krummel, Paul B.; Lunder, Chris Rene; Mühle, Jens; O'doherty, Simon; Prinn, Ronald G.; Reimann, Stefan; Vimont, Isaac; Wang, Hsiang; Weiss, Ray F.; Young, Dickon

2024

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