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Effect of Long-Range Transported Fire Aerosols on Cloud Condensation Nuclei Concentrations and Cloud Properties at High Latitudes

Kommula, Snehitha M.; Buchholz, Angela; Gramlich, Yvette; Mielonen, Tero; Hao, L.; Pullinen, Iida; Vettikkat, Lejish; Ylisirniö, A.; Joutsensaari, J.; Schobesberger, Siegfried; Tiitta, P; Leskinen, Ari; Heslin-Rees, Dominic; Haslett, S. L.; Siegel, Karolina; Lunder, Chris Rene; Zieger, Paul; Krejci, Radovan; Romakkaniemi, Sami; Mohr, C.; Virtanen, Annele

Active vegetation fires in south-eastern (SE) Europe resulted in a notable increase in the number concentration of aerosols and cloud condensation nuclei (CCN) particles at two high latitude locations—the SMEAR IV station in Kuopio, Finland, and the Zeppelin Observatory in Svalbard, high Arctic. During the fire episode aerosol hygroscopicity κ slightly increased at SMEAR IV and at the Zeppelin Observatory κ decreased. Despite increased κ in high CCN conditions at SMEAR IV, the aerosol activation diameter increased due to the decreased supersaturation with an increase in aerosol loading. In addition, at SMEAR IV during the fire episode, in situ measured cloud droplet number concentration (CDNC) increased by a factor of ∼7 as compared to non-fire periods which was in good agreement with the satellite observations (MODIS, Terra). Results from this study show the importance of SE European fires for cloud properties and radiative forcing in high latitudes.

American Geophysical Union (AGU)

2024

Recent advances and current challenges of new approach methodologies in developmental and adult neurotoxicity testing

Serafini, Melania Maria; Sepheri, Sara; Midali, Miriam; Stinckens, Marth; Biesiekierska, Marta; Wolniakowska, Anna; Gatzios, Alexandra; Rundén-Pran, Elise; Reszka, Edyta; Marinovich, Marina; Vanhaecke, Tamara; Roszak, Joanna; Viviani, Barbara; Tanima, SenGupta

Adult neurotoxicity (ANT) and developmental neurotoxicity (DNT) assessments aim to understand the adverse effects and underlying mechanisms of toxicants on the human nervous system. In recent years, there has been an increasing focus on the so-called new approach methodologies (NAMs). The Organization for Economic Co-operation and Development (OECD), together with European and American regulatory agencies, promote the use of validated alternative test systems, but to date, guidelines for regulatory DNT and ANT assessment rely primarily on classical animal testing. Alternative methods include both non-animal approaches and test systems on non-vertebrates (e.g., nematodes) or non-mammals (e.g., fish). Therefore, this review summarizes the recent advances of NAMs focusing on ANT and DNT and highlights the potential and current critical issues for the full implementation of these methods in the future. The status of the DNT in vitro battery (DNT IVB) is also reviewed as a first step of NAMs for the assessment of neurotoxicity in the regulatory context. Critical issues such as (i) the need for test batteries and method integration (from in silico and in vitro to in vivo alternatives, e.g., zebrafish, C. elegans) requiring interdisciplinarity to manage complexity, (ii) interlaboratory transferability, and (iii) the urgent need for method validation are discussed.

Springer

2024

The Greenhouse Gas Budget of Terrestrial Ecosystems in East Asia Since 2000

Wang, Xuhui; Gao, Yuanyi; Jeong, Sujong; Ito, Akihiko; Bastos, Ana; Poulter, Benjamin; Wang, Yilong; Ciais, Philippe; Tian, Hanqin; Yuan, Wenping; Chandra, Naveen; Chevallier, Frédéric; Fan, Lei; Hong, Songbai; Lauerwald, Ronny; Li, Wei; Lin, Zhengyang; Pan, Naiqing; Patra, Prabir K.; Peng, Shushi; Ran, Lishan; Sang, Yuxing; Sitch, Stephen; Takashi, Maki; Thompson, Rona Louise; Wang, Chenzhi; Wang, Kai; Wang, Tao; Xi, Yi; Xu, Liang; Yan, Yanzi; Yun, Jeongmin; Zhang, Yao; Zhang, Yuzhong; Zhang, Zhen; Zheng, Bo; Zhou, Feng; Tao, Shu; Canadell, Josep G.; Piao, Shilong

American Geophysical Union (AGU)

2024

Modelled sources of airborne microplastics collected at a remote Southern Hemisphere site

Aves, Alex; Ruffell, Helena; Evangeliou, Nikolaos; Gaw, Sally; Revell, Laura E.

Airborne microplastics have emerged in recent years as ubiquitous atmospheric pollutants. However, data from the Southern Hemisphere, and remote regions in particular, are sparse. Here, we report airborne microplastic deposition fluxes measured during a five-week sampling campaign at a remote site in the foothills of the Southern Alps of New Zealand. Samples were collected over 24-hour periods for the first week and for 7-day periods thereafter. On average, atmospheric microplastic (MP) deposition fluxes were six times larger during the 24-hour sampling periods (150 MP m−2 day−1) than during the 7-day sampling periods (26 MP m−2 day−1), highlighting the importance of sampling frequency and deposition collector design to limit particle resuspension. Previous studies, many of which used weekly sampling frequencies or longer, may have substantially underestimated atmospheric microplastic deposition fluxes, depending on the study design. To identify likely sources of deposited microplastics, we performed simulations with a global dispersion model coupled with an emissions inventory of airborne microplastics. Modelled deposition fluxes are in good agreement with observations, highlighting the potential for this method in tracing sources of deposited microplastics globally. Modelling indicates that sea-spray was the dominant source when microplastics underwent long-range atmospheric transport, with a small contribution from road dust.

Elsevier

2024

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

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