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Evaluation of multidecadal high-resolution atmospheric chemistry-transport modelling for exposure assessments in the continental Nordic countries

Frohn, Lise Marie; Geels, Camilla; Andersen, Christopher; Andersson, Camilla; Bennet, Cecilia; Christensen, Jesper H.; Im, Ulas; Karvosenoja, Niko; Kukkonen, Jaakko; Lopez-Aparicio, Susana; Nielsen, Ole-Kenneth; Palamarchuk, Yuliia; Paunu, Ville-Veikko; Plejdrup, Marlene S.; Segersson, David; Sofiev, Mikhail; Brandt, Jørgen

2022

Carbon–nitrogen interactions in European forests and semi-natural vegetation – Part 1: Fluxes and budgets of carbon, nitrogen and greenhouse gases from ecosystem monitoring and modelling

Flechard, Chris R.; Ibrom, Andreas; Skiba, Ute; Vries, Wim de; Oijen, Marcel Van; Cameron, David R.; Dise, Nancy B.; Korhonen, Janne; Buchmann, Nina; Legout, Arnaud; Simpson, David; Sanz, Maria J.; Aubinet, Marc; Loustau, Denis; Montagnani, Leonardo; Neirynck, Johan; Janssens, Ivan A.; Pihlatie, Mari; Kiese, Ralf; Siemens, Jan; Francez, Andre-Jean; Augustin, Jurgen; Varlagin, Andrej; Olejnik, Janusz; Juszczak, Radoslaw; Aurela, Mika; Berveiller, Daniel; Chojnicki, Bogdan H.; Dämmgen, Urich; Delpierre, Nicolas; Djuricic, Vesna; Drewer, Julia; Dufrene, Eric; Eugster, Werner; Fauvel, Yannick; Fowler, David; Frumau, Arnoud; Granier, Andre; Gross, Patrick; Hamon, Yannick; Helfter, Carole; Hensen, Arjan; Horvath, Laszlo; Kitzler, Barbara; Kruijt, Bart; Kutsch, Werner; Lobo-do-Vale, Raquel; Lohila, Annalea; Longdoz, Bernard; Marek, Michal V.; Matteucci, Giorgio; Mitosinkova, Marta; Moreaux, Virginie; Neftel, Albrecht; Ourcival, Jean-Marc; Pilegaard, Kim; Pita, Gabriel; Sanz, Francisco; Schjoerring, Jan K.; Sebastià, Maria-Teresa; Tang, Y. Sim; Uggerud, Hilde Thelle; Urbaniak, Marek; Dijk, Netty van; Vesala, Timo; Vidic, Sonja; Vincke, Caroline; Weidinger, Tamas; Sechmeister-Boltenstern, Sophie; Butterbach-Bahl, Klaus; Nemitz, Eiko; Sutton, Mark A.

The impact of atmospheric reactive nitrogen (Nr) deposition on carbon (C) sequestration in soils and biomass of unfertilized, natural, semi-natural and forest ecosystems has been much debated. Many previous results of this dC∕dN response were based on changes in carbon stocks from periodical soil and ecosystem inventories, associated with estimates of Nr deposition obtained from large-scale chemical transport models. This study and a companion paper (Flechard et al., 2020) strive to reduce uncertainties of N effects on C sequestration by linking multi-annual gross and net ecosystem productivity estimates from 40 eddy covariance flux towers across Europe to local measurement-based estimates of dry and wet Nr deposition from a dedicated collocated monitoring network. To identify possible ecological drivers and processes affecting the interplay between C and Nr inputs and losses, these data were also combined with in situ flux measurements of NO, N2O and CH4 fluxes; soil NO−3

leaching sampling; and results of soil incubation experiments for N and greenhouse gas (GHG) emissions, as well as surveys of available data from online databases and from the literature, together with forest ecosystem (BASFOR) modelling.

Multi-year averages of net ecosystem productivity (NEP) in forests ranged from −70 to 826 g C m−2 yr−1 at total wet + dry inorganic Nr deposition rates (Ndep) of 0.3 to 4.3 g N m−2 yr−1 and from −4 to 361 g C m−2 yr−1 at Ndep rates of 0.1 to 3.1 g N m−2 yr−1 in short semi-natural vegetation (moorlands, wetlands and unfertilized extensively managed grasslands). The GHG budgets of the forests were strongly dominated by CO2 exchange, while CH4 and N2O exchange comprised a larger proportion of the GHG balance in short semi-natural vegetation. Uncertainties in elemental budgets were much larger for nitrogen than carbon, especially at sites with elevated Ndep where Nr leaching losses were also very large, and compounded by the lack of reliable data on organic nitrogen and N2 losses by denitrification. Nitrogen losses in the form of NO, N2O and especially NO−3
were on average 27 % (range 6 %–54 %) of Ndep at sites with Ndep < 1 g N m−2 yr−1 versus 65 % (range 35 %–85 %) for Ndep > 3 g N m−2 yr−1. Such large levels of Nr loss likely indicate that different stages of N saturation occurred at a number of sites. The joint analysis of the C and N budgets provided further hints that N saturation could be detected in altered patterns of forest growth. Net ecosystem productivity increased with Nr deposition up to 2–2.5 g N m−2 yr−1, with large scatter associated with a wide range in carbon sequestration efficiency (CSE, defined as the NEP ∕ GPP ratio). At elevated Ndep levels (> 2.5 g N m−2 yr−1), where inorganic Nr losses were also increasingly large, NEP levelled off and then decreased. The apparent increase in NEP at low to intermediate Ndep levels was partly the result of geographical cross-correlations between Ndep and climate, indicating that the actual mean dC∕dN response at individual sites was significantly lower than would be suggested by a simple, straightforward regression of NEP vs. Ndep.

2020

Understanding of European cold extremes, sudden stratospheric warming, and Siberian snow accumulation in the winter of 2017/18

Lü, Zhuozhuo; Li, Fei; Orsolini, Yvan; Gao, Yongqi; He, Shengping

It is unclear whether the Eurasian snow plays a role in the tropospheric driving of sudden stratospheric warming (SSW). The major SSW event of February 2018 is analyzed using reanalysis datasets. Characterized by predominant planetary waves of zonal wave 2, the SSW developed into a vortex split via wave–mean flow interaction. In the following two weeks, the downward migration of zonal-mean zonal wind anomalies was accompanied by a significant transition to the negative phase of the North Atlantic Oscillation, leading to extensive cold extremes across Europe. Here, we demonstrate that anomalous Siberian snow accumulation could have played an important role in the 2018 SSW occurrence. In the 2017/18 winter, snow depths over Siberia were much higher than normal. A lead–lag correlation analysis shows that the positive fluctuating snow depth anomalies, leading to intensified “cold domes” over eastern Siberia (i.e., in a region where the climatological upward planetary waves maximize), precede enhanced wave-2 pulses of meridional heat fluxes (100 hPa) by 7–8 days. The snow–SSW linkage over 2003–19 is further investigated, and some common traits among three split events are found. These include a time lag of about one week between the maximum anomalies of snow depth and wave-2 pulses (100 hPa), high sea level pressure favored by anomalous snowpack, and a ridge anchoring over Siberia as precursor of the splits. The role of tropospheric ridges over Alaska and the Urals in the wave-2 enhancement and the role of Arctic sea ice loss in Siberian snow accumulation are also discussed.

2020

Temporal Trends of Organochlorine and Perfluorinated Contaminants in a Terrestrial Raptor in Northern Europe Over 34 years (1986–2019)

Bustnes, Jan Ove; Bårdsen, Bård-Jørgen; Herzke, Dorte; Bangjord, Georg; Bourgeon, Sophie; Fritsch, Clémentine; Eulaers, Igor

Fourteen legacy organochlorine (OC) contaminants and 12 perfluoroalkyl substances (PFASs) were measured in eggs of tawny owls (Strix alueco) in central Norway (1986–2019). We expected OCs to have reached stable equilibrium levels due to bans, and that recent phase-out of some PFASs would have slowed the increase of these compounds. ∑OC comprised on average approximately 92% of the measured compounds, whereas ∑PFAS accounted for approximately 8%. However, whereas the ∑OC to ∑PFAS ratio was approximately 60 in the first 5 years of the study, it was only approximately 11 in the last 5 years. Both OC pesticides and polychlorinated biphenyls (PCBs) showed substantial declines over the study period (~85%–98%): hexachlorocyclohexanes and chlordanes seemed to be levelling off, whereas p,p′-dichlorodiphenyldichloroethylene (p,p′-DDE) and hexachlororbenzene (HCB), and most PCB congeners still seemed to decline at a more or less constant rate. While the concentration of perfluorooctane sulfonic acid (PFOS), the dominating PFAS, was reduced by approximately 43%, other perfluorinated sulfonates (PFSAs) showed only minor changes. Moreover, the median concentrations of seven perfluorinated carboxylic acids (PFCAs) increased approximately five-fold over the study period. Perfluorononanoic acid and perfluoroundecanoate acid, however, seemed to be levelling off in recent years. In contrast, perfluorododecanoic acid, perfluorodecanoate acid, perfluorotridecanoic acid, and perfluorotetradecanoic acid seemed to increase more or less linearily. Finally, perfluorooctanoic acid (PFOA) was increasingly likely to be detected over the study period. Hence, most legacy OCs and PFOS have not reached a lower threshold with stable background levels, and voluntary elimination of perfluoroalkyl carboxylates still has not resulted in declining levels in tawny owls in central Norway.

2022

Polybrominated diphenyl ethers in type 2 diabetes mellitus cases and controls: Repeated measurements prior to and after diagnosis

Charles, Dolley; Berg, Vivian; Nøst, Therese Haugdahl; Wilsgaard, Tom; Bergdahl, Ingvar A.; Huber, Sandra; Ayotte, Pierre; Averina, Maria; Sandanger, Torkjel M; Rylander, Karin Charlotta Maria

Background Previous studies have reported associations between certain persistent organic pollutants (POPs) and type 2 diabetes mellitus (T2DM). Polybrominated diphenyl ethers (PBDEs) are a class of POPs that are found in increasing concentrations in humans. Although obesity is a known risk factor for T2DM and PBDEs are fat-soluble, very few studies have investigated associations between PBDEs and T2DM. No longitudinal studies have assessed associations between repeated measurements of PBDE and T2DM in the same individuals and compared time trends of PBDEs in T2DM cases and controls. Objectives To investigate associations between pre- and post-diagnostic measurements of PBDEs and T2DM and to compare time trends of PBDEs in T2DM cases and controls. Methods Questionnaire data and serum samples from participants in the Tromsø Study were used to conduct a longitudinal nested case-control study among 116 T2DM cases and 139 controls. All included study participants had three pre-diagnostic blood samples (collected before T2DM diagnosis in cases), and up to two post-diagnostic samples after T2DM diagnosis. We used logistic regression models to investigate pre- and post-diagnostic associations between PBDEs and T2DM, and linear mixed-effect models to assess time trends of PBDEs in T2DM cases and controls. Results We observed no substantial pre- or post-diagnostic associations between any of the PBDEs and T2DM, except for BDE-154 at one of the post-diagnostic time-points (OR = 1.65, 95% CI: 1.00, 2.71). The overall time trends of PBDE concentrations were similar for cases and controls. Discussion The study did not support PBDEs increasing the odds of T2DM, prior to or after T2DM diagnosis. T2DM status did not influence the time trends of PBDE concentrations.

2023

Ecosystem specific accumulation of organohalogenated compounds: A comparison between adjacent freshwater and terrestrial avian predators

Bustnes, Jan Ove; Bårdsen, Bård-Jørgen; Herzke, Dorte; Bangjord, Georg; Bourgeon, Sophie; Fritsch, Clémentine; Eulaers, Igor

Insight into processes determining the exposure of organohalogenated contaminants (OHCs) in wildlife might be gained from comparing predators in different ecosystems. This study compared two avian predator species with similar food chain lengths: the goldeneye duck (Bucephala clangula) and the tawny owl (Strix aluco) breeding in adjacent freshwater- and terrestrial ecosystems in central Norway. We measured lipophilic organochlorines (OCs) and protein-bound perfluorinated substances (PFASs) in eggs of the two species over 21 years (1999–2019). Across years, the proportional distribution of OCs (∼90% of the ΣOHC load) relative to PFASs (∼10%) was similar in the two species. Moreover, ΣOC concentrations were similar between the species, but PFAS compounds were 2–12 times higher in the goldeneyes than in tawny owls. OC-pesticides dominated in tawny owls (∼60% of ΣOC), whereas persistent polychlorinated biphenyl (PCBs) congeners were the main OC components in goldeneyes (∼70% of ΣOC). The lipid-normalized concentrations of most OC-pesticides and the less persistent PCB101 declined significantly in both species. Hexachlorobenzene (HCB), p,p’-dichlorodiphenyldichloroethylene (p,p’-DDE), and more persistent PCBs decreased in tawny owls, while they tended to increase in goldeneyes. The increase in HCB was particulary robust. Among the PFASs, contrasted temporal trends were found across the species for four out of 11 compounds: PFOS declined while most perfluorocarboxylic acids (PFCAs) increased in tawny owls. In contrast, most PFASs were stable in goldeneyes. Moreover, there was no annual covariance between the OHC exposure in the two species: i.e., high concentrations in one species in a given year did not translate into high concentrations in the other. Hence, the two avian predators in adjacent ecosystems seem to be subject to different processes determining the OHC exposure, probably related to variation in diet and climate, long-range transport of different contaminants, and emissions of pollution locally.

2022

Impact of 3D cloud structures on the atmospheric trace gas products from UV–Vis sounders – Part 3: Bias estimate using synthetic and observational data

Kylling, Arve; Emde, Claudia; Yu, Huan; Roozendael, Michel van; Stebel, Kerstin; Veihelmann, Ben; Mayer, Bernhard

Three-dimensional (3D) cloud structures may impact atmospheric trace gas products from ultraviolet–visible (UV–Vis) sounders. We used synthetic and observational data to identify and quantify possible cloud-related bias in NO2 tropospheric vertical column density (TVCD). The synthetic data were based on high-resolution large eddy simulations which were input to a 3D radiative transfer model. The simulated visible spectra for low-earth-orbiting and geostationary geometries were analysed with standard retrieval methods and cloud correction schemes that are employed in operational NO2 satellite products. For the observational data, the NO2 products from the TROPOspheric Monitoring Instrument (TROPOMI) were used, while the Visible Infrared Imaging Radiometer Suite (VIIRS) provided high-spatial-resolution cloud and radiance data. NO2 profile shape, cloud shadow fraction, cloud top height, cloud optical depth, and solar zenith and viewing angles were identified as the metrics being the most important in identifying 3D cloud impacts on NO2 TVCD retrievals. For a solar zenith angle less than about 40∘ the synthetic data show that the NO2 TVCD bias is typically below 10 %, while for larger solar zenith angles the NO2 TVCD is low-biased by tens of percent. The horizontal variability of NO2 and differences in TROPOMI and VIIRS overpass times make it challenging to identify a similar bias in the observational data. However, for optically thick clouds above 3000 m, a low bias appears to be present in the observational data.

2022

On the tuning of atmospheric inverse methods: comparisons with the European Tracer Experiment (ETEX) and Chernobyl datasets using the atmospheric transport model FLEXPART

Šmídl, Václav; Evangeliou, Nikolaos; Stohl, Andreas

Estimation of the temporal profile of an atmospheric release, also called the source term, is an important problem in environmental sciences. The problem can be formalized as a linear inverse problem wherein the unknown source term is optimized to minimize the difference between the measurements and the corresponding model predictions. The problem is typically ill-posed due to low sensor coverage of a release and due to uncertainties, e.g., in measurements or atmospheric transport modeling; hence, all state-of-the-art methods are based on some form of regularization of the problem using additional information. We consider two kinds of additional information: the prior source term, also known as the first guess, and regularization parameters for the shape of the source term. While the first guess is based on information independent of the measurements, such as the physics of the potential release or previous estimations, the regularization parameters are often selected by the designers of the optimization procedure. In this paper, we provide a sensitivity study of two inverse methodologies on the choice of the prior source term and regularization parameters of the methods. The sensitivity is studied in two cases: data from the European Tracer Experiment (ETEX) using FLEXPART v8.1 and the caesium-134 and caesium-137 dataset from the Chernobyl accident using FLEXPART v10.3.

2020

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.

2024

Method Development to Assess the Ventilated and Nonventilated Sources of Indoor Dust Deposits, Applied in a Museum

Grøntoft, Terje; Buchwald-Ziecina, Oliwia

A method was developed to analytically distinguish between the ventilated (v) and nonventilated (nv) fractions of water-soluble ions in deposits of particle indoors. The indicative method was based on low-cost passive outdoor and indoor sampling of the particle and ion deposits and NO2 gas and analysis of the regression values and residuals of the correlations between these parameters. The method was applied to measurements in the Pieskowa Skała Castle Museum in Poland. A dominating source of “soil and building dust” was indicated all year round, probably partly from renovation works of the castle, with larger total infiltration in the winter–spring (W-S) but with a higher proportion of ventilation ingress in the summer–autumn (S-A). About 60%–80%, by mass, of the water-soluble ions in the soil and building dust were calcium and probably some magnesium bicarbonate (Ca(HCO3)2, Mg(HCO3)2) and about 10%–20% sulfates (SO4−−) with calcium (Ca++) and several other cations. The other main source of the ion deposits was indicated to be air pollution, with chloride (Cl−), sulfate (SO4−−), and nitrate (NO3−), from outdoor combustion sources, like traffic, residential heating, and industry. These were mainly v from outdoors in the colder parts of the year, but also to the more open locations in the S-A. A small source of nv sulfate (SO4−−) was identified inside two showcases in the S-A. The study showed good enclosure protection of the museum objects against exposure to particle pollution, but also the need to avoid the trapping of particle pollution inside showcases or closed rooms. The identification of the probable different amounts and sources of v and nv ions in the castle aided preventive actions to reduce the pollution exposure.

2024

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; Jones, Dean P.; Barupal, Dinesh Kumar; Bowden, John; Rostkowski, Pawel Marian; Pennell, Kurt D.; 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

Environmental dose-response functions of silk and paper exposed in museums.

Grøntoft, Terje; Hallett, Kathryn; Blades, Nigel

This paper reports 1 year of data of the environments and changes in the molecular weight of silk and the degree of polymerization of sensitive paper measured externally and indoors in 10 European museums, and the dose-response functions that were obtained by statistical analysis of this data. The measurements were performed in the EU FP5 project Master (EVK-CT-2002-00093). The work provides documentation of deterioration of silk by NO2 and O3, and alternatively in combination with UV radiation. The indoor deterioration of the silk was only observed in one location with high UV radiation. The indoor deterioration of sensitive paper correlated with the UV radiation, the concentrations of NO2 and O3, and in addition with an SO2 concentration of 4 µgm−3 and a formic acid concentration of 50 µgm−3 in two different locations. If the observed dose-response effects are linear to lower doses and longer exposure times, then the lifetime to intolerable deterioration of the paper and silk would be 6–7 times longer overall in the enclosures than in the galleries.

2024

Impact of genetic polymorphisms in kinetochore and spindle assembly genes on chromosomal aberration frequency in healthy humans

Niazi, Yasmeen; Thomsen, Hauke; Smolkova, Bozena; Vodickova, Ludmila; Vodenkova, Sona; Kroupa, Michal; Vymetalkova, Veronika; Kazimirova, Alena; Barancokova, Magdalena; Volkovova, Katarina; Hoffmann, Per; Nöthen, Markus M.; Dusinska, Maria; Musak, Ludovit; Vodicka, Pavel; Hemminki, Kari; Försti, Asta

2020

Polycyclic Aromatic Hydrocarbons Not Declining in Arctic Air Despite Global Emission Reduction

Yu, Yong; Katsoyiannis, Athanasios A.; Bohlin-Nizzetto, Pernilla; Brorström-Lundén, Eva; Ma, Jianmin; Zhao, Yuan; Wu, Zhiyong; Tych, Wlodzimierz; Mindham, David; Sverko, Ed; Barresi, Enzo; Dryfhout-Clark, Helena; Fellin, Phil; Hung, Hayley

Two decades of atmospheric measurements of polycyclic aromatic hydrocarbons (PAHs) were conducted at three Arctic sites, i.e., Alert, Canada; Zeppelin, Svalbard; and Pallas, Finland. PAH concentrations decrease with increasing latitude in the order of Pallas > Zeppelin > Alert. Forest fire was identified as an important contributing source. Three representative PAHs, phenanthrene (PHE), pyrene (PYR), and benzo[a]pyrene (BaP) were selected for the assessment of their long-term trends. Significant decline of these PAHs was not observed contradicting the expected decline due to PAH emission reductions. A global 3-D transport model was employed to simulate the concentrations of these three PAHs at the three sites. The model predicted that warming in the Arctic would cause the air concentrations of PHE and PYR to increase in the Arctic atmosphere, while that of BaP, which tends to be particle-bound, is less affected by temperature. The expected decline due to the reduction of global PAH emissions is offset by the increment of volatilization caused by warming. This work shows that this phenomenon may affect the environmental occurrence of other anthropogenic substances, such as more volatile flame retardants and pesticides.

2019

Anthropogenic Carbon Monoxide Emissions During 2014–2020 in China Constrained by In Situ Ground Observations

Jia, Mengwei; Jiang, Fei; Evangeliou, Nikolaos; Eckhardt, Sabine; Stohl, Andreas; Huang, Xin; Sheng, Yang; Feng, Shuzhuang; He, Wei; Wang, Hengmao; Wu, Mousong; Ju, Weimin; Ding, Aijun

2025

Anthropogenic compounds in the northernmost Atlantic puffin population

Underwood, Arin; Descamps, Sebastien; Sagerup, Kjetil; Herzke, Dorte; Gabrielsen, Geir W.

Contamination by organic pollutants, even in remote regions, poses a growing threat to wildlife, including seabirds. However, for many seabirds breeding at high latitudes, both the extent and nature of contaminant exposure remain largely unknown. This study aimed to identify the persistent organic pollutants (POPs) present in the Svalbard Atlantic puffin Fratercula arctica at the northern limit of its range. We also compare contaminant concentrations with those found in other species breeding on Svalbard and in puffin colonies further south. The Svalbard puffins were found to be contaminated by organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs), and per- and polyfluoroalkyl substances (PFAS). No significant sex difference was found. OCPs, PCBs and/or PFASs concentrations in Svalbard puffins were comparable to those of Brünnich's guillemots Uria lomvia, black guillemots Cepphus grylle, and/or little auks Alle alle, but lower than in glaucous gulls Larus hyperboreus. PFAS concentrations were also lower than in black-legged kittiwakes Rissa tridactyla. OCP and PCB concentrations were lower on Svalbard than in puffin colonies further south. This study is the first to document PFAS concentrations in puffins, therefore it remains unknown whether PFAS levels were also lower on Svalbard than further south. These comparisons should be interpreted with caution, as data for different species or colonies were collected in different years, and contaminant levels vary over time. The current contaminant concentrations indicate that Svalbard puffins are still at low risk for biological effects, but continued monitoring is needed to assess potential future changes.

2025

Real-time UV index retrieval in Europe using Earth observation-based techniques: system description and quality assessment

Kosmopoulos, Panagiotis G.; Kazadzis, Stelios; Schmalwieser, Alois W.; Raptis, Panagiotis I.; Papachristopoulou, Kyriakoula; Fountoulakis, Ilias; Masoom, Akriti; Bais, Alkiviadis F.; Bilbao, Julia; Blumthaler, Mario; Kreuter, Axel; Siani, Anna Maria; Eleftheratos, Kostas; Topaloglou, Chrystanthi; Gröbner, Julian; Johnsen, Bjørn; Svendby, Tove Marit; Vilaplana, Jose Manuel; Doppler, Lionel; Webb, Ann R; Khazova, Marina; Backer, Hugo De; Heikkilä, Anu; Lakkala, Kaisa; Jaroslawski, Janusz; Meleti, Charikleia; Diémoz, Henri; Hülsen, Gregor; Klotz, Barbara; Rimmer, John; Kontoes, Charalampos

This study introduces an Earth observation (EO)-based system which is capable of operationally estimating and continuously monitoring the ultraviolet index (UVI) in Europe. UVIOS (i.e., UV-Index Operating System) exploits a synergy of radiative transfer models with high-performance computing and EO data from satellites (Meteosat Second Generation and Meteorological Operational Satellite-B) and retrieval processes (Tropospheric Emission Monitoring Internet Service, Copernicus Atmosphere Monitoring Service and the Global Land Service). It provides a near-real-time nowcasting and short-term forecasting service for UV radiation over Europe. The main atmospheric inputs for the UVI simulations include ozone, clouds and aerosols, while the impacts of ground elevation and surface albedo are also taken into account. The UVIOS output is the UVI at high spatial and temporal resolution (5 km and 15 min, respectively) for Europe (i.e., 1.5 million pixels) in real time. The UVI is empirically related to biologically important UV dose rates, and the reliability of this EO-based solution was verified against ground-based measurements from 17 stations across Europe. Stations are equipped with spectral, broadband or multi-filter instruments and cover a range of topographic and atmospheric conditions. A period of over 1 year of forecasted 15 min retrievals under all-sky conditions was compared with the ground-based measurements. UVIOS forecasts were within ±0.5 of the measured UVI for at least 70 % of the data compared at all stations. For clear-sky conditions the agreement was better than 0.5 UVI for 80 % of the data. A sensitivity analysis of EO inputs and UVIOS outputs was performed in order to quantify the level of uncertainty in the derived products and to identify the covariance between the accuracy of the output and the spatial and temporal resolution and the quality of the inputs. Overall, UVIOS slightly overestimated the UVI due to observational uncertainties in inputs of cloud and aerosol. This service will hopefully contribute to EO capabilities and will assist the provision of operational early warning systems that will help raise awareness among European Union citizens of the health implications of high UVI doses.

2021

Is Glacial Meltwater a Secondary Source of Legacy Contaminants to Arctic Coastal Food Webs?

Mcgovern, Maeve; Warner, Nicholas Alexander; Borgå, Katrine; Evenset, Anita; Carlsson, Pernilla; Skogsberg, Emelie; Søreide, Janne; Ruus, Anders; Christensen, Guttorm; Poste, Amanda

Climate change-driven increases in air and sea temperatures are rapidly thawing the Arctic cryosphere with potential for remobilization and accumulation of legacy persistent organic pollutants (POPs) in adjacent coastal food webs. Here, we present concentrations of selected POPs in zooplankton (spatially and seasonally), as well as zoobenthos and sculpin (spatially) from Isfjorden, Svalbard. Herbivorous zooplankton contaminant concentrations were highest in May [e.g., ∑polychlorinated biphenyls (8PCB); 4.43, 95% CI: 2.72–6.3 ng/g lipid weight], coinciding with the final stages of the spring phytoplankton bloom, and lowest in August (∑8PCB; 1.6, 95% CI: 1.29–1.92 ng/g lipid weight) when zooplankton lipid content was highest, and the fjord was heavily impacted by sediment-laden terrestrial inputs. Slightly increasing concentrations of α-hexachlorocyclohexane (α-HCH) in zooplankton from June (1.18, 95% CI: 1.06–1.29 ng/g lipid weight) to August (1.57, 95% CI: 1.44–1.71 ng/g lipid weight), alongside a higher percentage of α-HCH enantiomeric fractions closer to racemic ranges, indicate that glacial meltwater is a secondary source of α-HCH to fjord zooplankton in late summer. Except for α-HCH, terrestrial inputs were generally associated with reduced POP concentrations in zooplankton, suggesting that increased glacial melt is not likely to significantly increase exposure of legacy POPs in coastal fauna.

2022

Evaluation and optimization of ICOS atmosphere station data as part of the labeling process

Yver-Kwok, Camille; Philippon, Camille; Bergamaschi, Peter; Biermann, Tobias; Calzolari, Francescopiero; Chen, Huilin; Conil, Sébastien; Cristofanelli, Paolo; Delmotte, Marc; Hatakka, Juha; Heliasz, Michal; Hermansen, Ove; Kominkova, Katerina; Kubistin, Dagmar; Kumps, Nicolas; Laurent, Olivier; Laurila, Tuomas; Lehner, Irene; Levula, Janne; Lindauer, Matthias; Lopez, Morgan; Mammarella, Ivan; Manca, Giovanni; Marklund, Per; Metzger, Jean-Marc; Mölder, Meelis; Platt, Stephen Matthew; Ramonet, Michel; Rivier, Leonard; Scheeren, Bert; Sha, Mahesh Kumar; Smith, Paul; Steinbacher, Martin; Vitkova, Gabriela; Wyss, Simon

The Integrated Carbon Observation System (ICOS) is a pan-European research infrastructure which provides harmonized and high-precision scientific data on the carbon cycle and the greenhouse gas budget. All stations have to undergo a rigorous assessment before being labeled, i.e., receiving approval to join the network. In this paper, we present the labeling process for the ICOS atmosphere network through the 23 stations that were labeled between November 2017 and November 2019. We describe the labeling steps, as well as the quality controls, used to verify that the ICOS data (CO2, CH4, CO and meteorological measurements) attain the expected quality level defined within ICOS. To ensure the quality of the greenhouse gas data, three to four calibration gases and two target gases are measured: one target two to three times a day, the other gases twice a month. The data are verified on a weekly basis, and tests on the station sampling lines are performed twice a year. From these high-quality data, we conclude that regular calibrations of the CO2, CH4 and CO analyzers used here (twice a month) are important in particular for carbon monoxide (CO) due to the analyzer's variability and that reducing the number of calibration injections (from four to three) in a calibration sequence is possible, saving gas and extending the calibration gas lifespan. We also show that currently, the on-site water vapor correction test does not deliver quantitative results possibly due to environmental factors. Thus the use of a drying system is strongly recommended. Finally, the mandatory regular intake line tests are shown to be useful in detecting artifacts and leaks, as shown here via three different examples at the stations.

2021

Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude.

The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires.

In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and coastal areas. The formation of 23, 27 and 27 %, respectively of, ammonium, nitrate and sulfate aerosols is due to the emissions within the marine and coastal area.

2018

UV-degradation is a key driver of the fate and impacts of marine plastics. How can laboratory experiments be designed to effectively inform risk assessment?

Hernandez, Laura M.; Howarth-Forster, Lucy; Sørensen, Lisbet; Booth, Andrew Michael; Vidal, Alice; Tufenkji, Nathalie; Sempéré, Richard; Schmidt, Natascha

Marine plastic litter is subject to different abiotic and biotic forces that lead to its degradation, the main driver being UV-induced photodegradation. Since UV-exposure leads to both physical and chemical degradation of plastic, leading to a release of micro- and nanoplastics as well as leaching of chemicals and degradation products – it is expected to have radical impacts on plastics fate and effects in the marine environment. The number of laboratory studies investigating the mechanisms of plastic UV-degradation in seawater has increased significantly in the past 10 years, but are the exposures designed in a manner that allow observations to be extrapolated to environmental fate? Most studies to date focus on quantifying plastic fragmentation and surface changes, but is this relevant for impact assessments? Here, we provide a review of the current scientific literature on UV-degradation of plastic under marine conditions. Plastic fragmentation processes and surface changes as well as implications of UV-degradation of plastics on additive leaching and the toxicity of UV-weathered versus non-weathered plastics are highlighted. Furthermore, experimental set-ups are critically inspected and recommendations for future studies are issued.

2025

Mineral Dust Instantaneous Radiative Forcing in the Arctic

Kylling, Arve; Zwaaftink, Christine Groot; Stohl, Andreas

2018

Comparison of dust-layer heights from active and passive satellite sensors

Kylling, Arve; Vandenbussche, Sophie; Capelle, Virginie; Cuesta, Juan; Klüser, Lars; Lelli, Luca; Popp, Thomas; Stebel, Kerstin; Veefkind, Pepijn

Aerosol-layer height is essential for understanding the impact of aerosols on the climate system. As part of the European Space Agency Aerosol_cci project, aerosol-layer height as derived from passive thermal and solar satellite sensors measurements have been compared with aerosol-layer heights estimated from CALIOP measurements. The Aerosol_cci project targeted dust-type aerosol for this study. This ensures relatively unambiguous aerosol identification by the CALIOP processing chain. Dust-layer height was estimated from thermal IASI measurements using four different algorithms (from BIRA-IASB, DLR, LMD, LISA) and from solar GOME-2 (KNMI) and SCIAMACHY (IUP) measurements. Due to differences in overpass time of the various satellites, a trajectory model was used to move the CALIOP-derived dust heights in space and time to the IASI, GOME-2 and SCIAMACHY dust height pixels. It is not possible to construct a unique dust-layer height from the CALIOP data. Thus two CALIOP-derived layer heights were used: the cumulative extinction height defined as the height where the CALIOP extinction column is half of the total extinction column, and the geometric mean height, which is defined as the geometrical mean of the top and bottom heights of the dust layer. In statistical average over all IASI data there is a general tendency to a positive bias of 0.5–0.8 km against CALIOP extinction-weighted height for three of the four algorithms assessed, while the fourth algorithm has almost no bias. When comparing geometric mean height there is a shift of −0.5 km for all algorithms (getting close to zero for the three algorithms and turning negative for the fourth). The standard deviation of all algorithms is quite similar and ranges between 1.0 and 1.3 km. When looking at different conditions (day, night, land, ocean), there is more detail in variabilities (e.g. all algorithms overestimate more at night than during the day). For the solar sensors it is found that on average SCIAMACHY data are lower by −1.097 km (−0.961 km) compared to the CALIOP geometric mean (cumulative extinction) height, and GOME-2 data are lower by −1.393 km (−0.818 km).

2018

Copper Oxide Nanoparticles Stimulate the Immune Response and Decrease Antioxidant Defense in Mice After Six-Week Inhalation

Tulinska, Jana; Mikusova, Miroslava Lehotska; Liskova, Aurelia; Busova, Milena; Masanova, Vlasta; Uhnakova, Iveta; Rollerova, Eva; Alacova, Radka; Krivosikova, Zora; Wsolova, Ladislava; Dusinska, Maria; Horváthová, Mira; Szabova, Michaela; Lukan, Norbert; Stuchlikova, Martina; Kuba, Daniel; Vecera, Zbynek; Coufalik, Pavel; Krumal, Kamil; Alexa, Lukas; Vrlikova, Lucie; Buchtova, Marcela; Dumkova, Jana; Piler, Pavel; Thon, Vojtech; Mikuska, Pavel

Copper oxide nanoparticles (CuO NPs) are increasingly used in various industry sectors. Moreover, medical application of CuO NPs as antimicrobials also contributes to human exposure. Their toxicity, including toxicity to the immune system and blood, raises concerns, while information on their immunotoxicity is still very limited. The aim of our work was to evaluate the effects of CuO NPs (number concentration 1.40×106 particles/cm3, geometric mean diameter 20.4 nm) on immune/inflammatory response and antioxidant defense in mice exposed to 32.5 µg CuO/m3 continuously for 6 weeks. After six weeks of CuO NP inhalation, the content of copper in lungs and liver was significantly increased, while in kidneys, spleen, brain, and blood it was similar in exposed and control mice. Inhalation of CuO NPs caused a significant increase in proliferative response of T-lymphocytes after mitogenic stimulation and basal proliferative activity of splenocytes. CuO NPs significantly induced the production of IL-12p70, Th1-cytokine IFN-γ and Th2-cytokines IL-4, IL-5. Levels of TNF-α and IL-6 remained unchanged. Immune assays showed significantly suppressed phagocytic activity of granulocytes and slightly decreased respiratory burst. No significant differences in phagocytosis of monocytes were recorded. The percentage of CD3+, CD3+CD4+, CD3+CD8+, and CD3-CD19+ cell subsets in spleen, thymus, and lymph nodes did not differ between exposed and control animals. No changes in hematological parameters were found between the CuO NP exposed and control groups. The overall antioxidant protection status of the organism was expressed by evaluation of GSH and GSSG concentrations in blood samples. The experimental group exposed to CuO NPs showed a significant decrease in GSH concentration in comparison to the control group. In summary, our results indicate that sub-chronic inhalation of CuO NPs can cause undesired modulation of the immune response. Stimulation of adaptive immunity was indicated by activation of proliferation and secretion functions of lymphocytes. CuO NPs elicited pro-activation state of Th1 and Th2 lymphocytes in exposed mice. Innate immunity was affected by impaired phagocytic activity of granulocytes. Reduced glutathione was significantly decreased in mice exposed to CuO NPs.

2022

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