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Estimating methane emissions in the Arctic nations using surface observations from 2008 to 2019

Wittig, Sophie; Berchet, Antoine; Pison, Isabelle; Saunois, Marielle; Thanwerdas, Joel; Martinez, Adrien; Paris, Jean-Daniel; Machida, Toshinobu; Sasakawa, Motoki; Worthy, Doug E.J.; Lan, Xin; Thompson, Rona Louise; Sollum, Espen; Arshinov, Mikhail

The Arctic is a critical region in terms of global warming. Environmental changes are already progressing steadily in high northern latitudes, whereby, among other effects, a high potential for enhanced methane (CH4) emissions is induced. With CH4 being a potent greenhouse gas, additional emissions from Arctic regions may intensify global warming in the future through positive feedback. Various natural and anthropogenic sources are currently contributing to the Arctic's CH4 budget; however, the quantification of those emissions remains challenging. Assessing the amount of CH4 emissions in the Arctic and their contribution to the global budget still remains challenging. On the one hand, this is due to the difficulties in carrying out accurate measurements in such remote areas. Besides, large variations in the spatial distribution of methane sources and a poor understanding of the effects of ongoing changes in carbon decomposition, vegetation and hydrology also complicate the assessment. Therefore, the aim of this work is to reduce uncertainties in current bottom-up estimates of CH4 emissions as well as soil oxidation by implementing an inverse modelling approach in order to better quantify CH4 sources and sinks for the most recent years (2008 to 2019). More precisely, the objective is to detect occurring trends in the CH4 emissions and potential changes in seasonal emission patterns. The implementation of the inversion included footprint simulations obtained with the atmospheric transport model FLEXPART (FLEXible PARTicle dispersion model), various emission estimates from inventories and land surface models, and data on atmospheric CH4 concentrations from 41 surface observation sites in the Arctic nations. The results of the inversion showed that the majority of the CH4 sources currently present in high northern latitudes are poorly constrained by the existing observation network. Therefore, conclusions on trends and changes in the seasonal cycle could not be obtained for the corresponding CH4 sectors. Only CH4 fluxes from wetlands are adequately constrained, predominantly in North America. Within the period under study, wetland emissions show a slight negative trend in North America and a slight positive trend in East Eurasia. Overall, the estimated CH4 emissions are lower compared to the bottom-up estimates but higher than similar results from global inversions.

2023

Mercury isotope evidence for Arctic summertime re-emission of mercury from the cryosphere

Araujo, Beatriz Ferreira; Osterwalder, Stefan; Szponar, Natalie; Lee, Domenica; Petrova, Mariia V.; Pernov, Jakob Boyd; Ahmed, Shaddy; Heimbürger-Boavida, Lars-Eric; Laffont, Laure; Teisserenc, Roman; Tananaev, Nikita; Nordstrom, Claus; Magand, Olivier; Stupple, Geoff; Skov, Henrik; Steffen, Alexandra; Bergquist, Bridget; Pfaffhuber, Katrine Aspmo; Thomas, Jennie L.; Scheper, Simon; Petäjä, Tuukka; Dommergue, Aurélien; Sonke, Jeroen E.

During Arctic springtime, halogen radicals oxidize atmospheric elemental mercury (Hg0), which deposits to the cryosphere. This is followed by a summertime atmospheric Hg0 peak that is thought to result mostly from terrestrial Hg inputs to the Arctic Ocean, followed by photoreduction and emission to air. The large terrestrial Hg contribution to the Arctic Ocean and global atmosphere has raised concern over the potential release of permafrost Hg, via rivers and coastal erosion, with Arctic warming. Here we investigate Hg isotope variability of Arctic atmospheric, marine, and terrestrial Hg. We observe highly characteristic Hg isotope signatures during the summertime peak that reflect re-emission of Hg deposited to the cryosphere during spring. Air mass back trajectories support a cryospheric Hg emission source but no major terrestrial source. This implies that terrestrial Hg inputs to the Arctic Ocean remain in the marine ecosystem, without substantial loss to the global atmosphere, but with possible effects on food webs.

2022

Tropospheric ozone assessment report: Global ozone metrics for climate change, human health, and crop/ecosystem research

Lefohn, Allen S.; Malley, Christopher S.; Smith, Luther; Wells, Benjamin; Hazucha, Milan; Simon, Heather; Naik, Vaishali; Mills, Gina; Schultz, Martin G.; Paoletti, Elena; Marco, Alessandra De; Xu, Xiaobin; Zhang, Li; Wang, Tao; Neufeld, Howard S.; Musselman, Robert C.; Tarasick, David; Brauer, Michael; Feng, Zhaozhong; Tang, Haoye; Kobayashi, Kazuhiko; Sicard, Pierre; Solberg, Sverre; Gerosa, Giacomo

Assessment of spatial and temporal variation in the impacts of ozone on human health, vegetation, and climate requires appropriate metrics. A key component of the Tropospheric Ozone Assessment Report (TOAR) is the consistent calculation of these metrics at thousands of monitoring sites globally. Investigating temporal trends in these metrics required that the same statistical methods be applied across these ozone monitoring sites. The nonparametric Mann-Kendall test (for significant trends) and the Theil-Sen estimator (for estimating the magnitude of trend) were selected to provide robust methods across all sites. This paper provides the scientific underpinnings necessary to better understand the implications of and rationale for selecting a specific TOAR metric for assessing spatial and temporal variation in ozone for a particular impact. The rationale and underlying research evidence that influence the derivation of specific metrics are given. The form of 25 metrics (4 for model-measurement comparison, 5 for characterization of ozone in the free troposphere, 11 for human health impacts, and 5 for vegetation impacts) are described. Finally, this study categorizes health and vegetation exposure metrics based on the extent to which they are determined only by the highest hourly ozone levels, or by a wider range of values. The magnitude of the metrics is influenced by both the distribution of hourly average ozone concentrations at a site location, and the extent to which a particular metric is determined by relatively low, moderate, and high hourly ozone levels. Hence, for the same ozone time series, changes in the distribution of ozone concentrations can result in different changes in the magnitude and direction of trends for different metrics. Thus, dissimilar conclusions about the effect of changes in the drivers of ozone variability (e.g., precursor emissions) on health and vegetation exposure can result from the selection of different metrics.

2018

Estimating the air quality standard exceedance areas and the spatial representativeness of urban air quality stations applying microscale modelling

Martin, Fernando; Rodrigues, Vera; Santiago, José Luis; Sousa, Jorge; Stocker, Jenny R.; Russo, Felicita; Villani, Maria Gabriella; Tinarelli, G.; Barbero, D.; Jose, Roberto San; Pérez-Camanyo, Juan Luis; Santos, Gabriela Sousa; Tarrasón, Leonor; Bartzis, John; Sakellaris, I.; Horváth, Zoltán; Környei, László; Jurado, Xavier; Reiminger, N.; Masey, Nicola; Hamilton, Scott; Rivas, Esther; Cuvelier, Cournelius; Thunis, P.

This study builds upon the findings of a FAIRMODE intercomparison exercise conducted in a district of Antwerp, Belgium, where a comprehensive dataset of air pollutant measurements (air quality stations and passive samplers) was available. Long-term average NO2 concentrations at very high spatial resolution were estimated by several dispersion modelling systems (Martín et al., 2024) to investigate the ability of these to capture the detailed spatial distribution of NO2 concentrations at the microscale in urban environments. In this follow-up research, we extend the analysis by evaluating the capability of these modelling systems to predict the NO2 annual limit value exceedance areas (LVEAs) and spatial representativeness areas (SRAs) for NO₂ at two reference air quality stations. The different modelling approaches used are based on CFD, Lagrangian, Gaussian, and AI-driven models.
The different modelling approaches are generally good at predicting the LVEA and SRAs of urban air quality stations, although a small SRA (corresponding to low concentration tolerances or the traffic station) is more difficult to predict correctly. However, there are notable differences in performance among the modelling systems. Those based on CFD models seem to provide more consistent results predicting LVEAs and SRAs. Then, lower accuracy is obtained with AI-based systems, Lagrangian models, and Gaussian models with street canyon parameterizations. The Gaussian models with street-canyon parametrizations show significantly better results than models using simply a Gaussian dispersion parametrization.
Furthermore, little differences are observed in most of the statistical indicators corresponding to the LVEA and SRA estimates obtained from the unsteady full month CFD simulations compared to those from the scenario-based CFD simulation methodologies, but there are some noticeable differences in the LVEA or SRA (traffic station, 10 % tolerance) sizes. The number of scenarios does not seem to be relevant to the results. Different bias correction methodologies are explored.

2025

Can statistics of turbulent tracer dispersion be inferred from camera observations of SO2 in the ultraviolet? A modelling study

Kylling, Arve; Ardeshiri, Hamidreza; Cassiani, Massimo; Dinger, Anna Solvejg; Park, Soon-Young; Pisso, Ignacio; Schmidbauer, Josef Norbert; Stebel, Kerstin; Stohl, Andreas

Atmospheric turbulence and in particular its effect on tracer dispersion may be measured by cameras sensitive to the absorption of ultraviolet (UV) sunlight by sulfur dioxide (SO2), a gas that can be considered a passive tracer over short transport distances. We present a method to simulate UV camera measurements of SO2 with a 3D Monte Carlo radiative transfer model which takes input from a large eddy simulation (LES) of a SO2 plume released from a point source. From the simulated images the apparent absorbance and various plume density statistics (centre-line position, meandering, absolute and relative dispersion, and skewness) were calculated. These were compared with corresponding quantities obtained directly from the LES. Mean differences of centre-line position, absolute and relative dispersions, and skewness between the simulated images and the LES were generally found to be smaller than or about the voxel resolution of the LES. Furthermore, sensitivity studies were made to quantify how changes in solar azimuth and zenith angles, aerosol loading (background and in plume), and surface albedo impact the UV camera image plume statistics. Changing the values of these parameters within realistic limits has negligible effects on the centre-line position, meandering, absolute and relative dispersions, and skewness of the SO2 plume. Thus, we demonstrate that UV camera images of SO2 plumes may be used to derive plume statistics of relevance for the study of atmospheric turbulent dispersion.

2020

Fluorine Mass Balance, including Total Fluorine, Extractable Organic Fluorine, Oxidizable Precursors, and Target Per- and Polyfluoroalkyl Substances, in Pooled Human Serum from the Tromsø Population in 1986, 2007, and 2015

Cioni, Lara; Plassmann, Merle; Benskin, Jonathan P.; Coelho, Ana Carolina; Nøst, Therese Haugdahl; Rylander, Karin Charlotta Maria; Nikiforov, Vladimir; Sandanger, Torkjel Manning; Herzke, Dorte

Of the thousands of per- and polyfluoroalkyl substances (PFAS) known to exist, only a small fraction (≤1%) are commonly monitored in humans. This discrepancy has led to concerns that human exposure may be underestimated. Here, we address this problem by applying a comprehensive fluorine mass balance (FMB) approach, including total fluorine (TF), extractable organic fluorine (EOF), total oxidizable precursors (TOP), and selected target PFAS, to human serum samples collected over a period of 28 years (1986, 2007, and 2015) in Tromsø, Norway. While concentrations of TF did not change between sampling years, EOF was significantly higher in 1986 compared to 2007 and 2015. The ∑12PFAS concentrations were highest in 2007 compared to 1986 and 2015, and unidentified EOF (UEOF) decreased from 1986 (46%) to 2007 (10%) and then increased in 2015 (37%). While TF and EOF were not influenced by sex, women had higher UEOF compared to men, opposite to target PFAS. This is the first FMB in human serum to include TOP, and it suggests that precursors with >4 perfluorinated carbon atoms make a minor contribution to EOF (0–4%). Additional tools are therefore needed to identify substances contributing to the UEOF in human serum.

2023

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

2024

Feathers as integrated archives of environmental stress: Direct and indirect effects of metal exposure and dietary ecology on physiological stress in a terrestrial raptor

Hansen, Elisabeth; Bustnes, Jan Ove; Herzke, Dorte; Bangjord, Georg; Ballesteros, Manuel; Bårdsen, Bård-Jørgen; Bollinger, Eric; Schulz, Ralf; Eulaers, Igor; Bourgeon, Sophie

Metal pollution is a global environmental issue with adverse biological effects on wildlife. Long-term studies that span declines in metal emissions due to regulation, resulting in varying levels of environmental contamination, are therefore well-suited to investigate effects of toxic metals, while also facilitating robust analysis by incorporating fluctuating environmental conditions and food availability. Here, we examined a resident population of tawny owls in Norway between 1986 and 2019. Tail feathers from females were collected annually, resulting in over 1000 feathers. Each feather served as an archive of local environmental conditions during molt, including the presence of metals, and their dietary ecology, proxied by stable isotopes of nitrogen (δ15N) and carbon (δ13C), as well as corticosterone levels (CORTf), the primary avian glucocorticoid and a measure of physiological stress. We analyzed feathers to examine how exposure to toxic metal(loid)s (Al, As, Cd, Hg, and Pb) and variability in dietary proxies modulate CORTf. Using structural equation modelling, we found that increased Al concentrations and δ15N values, linked directly to increased CORTf. In opposite, we found that increased Hg concentrations and δ13C related to decreased CORTf concentrations. δ15N was indirectly linked to CORTf through Al and Hg, while δ13C was indirectly linked to CORTf through Hg. This supports our hypothesis that metal exposure and dietary ecology may individually or jointly influence physiological stress. Notably, our results suggest that dietary ecology has the potential to mediate the impact of metals on CORTf, highlighting the importance of considering multiple variables, direct and indirect effects, when assessing stress in wildlife. In conclusion, feathers represent an excellent non-destructive biomonitoring strategy in avian wildlife, providing valuable insights not easily accessible using other methods. Further research is warranted to fully comprehend implications of alterations in CORTf on the tawny owl's health and fitness.

2024

Regulatory practices on the genotoxicity testing of nanomaterials and outlook for the future

Andreoli, Cristina; Dusinska, Maria; Bossa, Cecilia; Battistelli, Chiara Laura; Silva, Maria João; Louro, Henriqueta

2025

Non-target and suspect characterisation of organic contaminants in Arctic air – Part 2: Application of a new tool for identification and prioritisation of chemicals of emerging Arctic concern in air

Röhler, Laura; Schlabach, Martin; Haglund, Peter; Breivik, Knut; Kallenborn, Roland; Bohlin-Nizzetto, Pernilla

The Norwegian Arctic possesses a unique environment for the detection of new potential chemicals of emerging Arctic concern (CEACs) due to remoteness, sparse population and the low number of local contamination sources. Hence, a contaminant present in Arctic air is still considered a priority indication for its environmental stability and environmental mobility. Today, legacy persistent organic pollutants (POPs) and related conventional environmental pollutants are already well-studied because of their identification as Arctic pollutants in the 1980s. Many of them are implemented and reported in various national and international monitoring activities including the Arctic Monitoring and Assessment Programme (AMAP). These standard monitoring schemes, however, are based on compound-specific quantitative analytical methods. Under such conditions, the possibility for the identification of hitherto unidentified contaminants is limited and random at best. Today, new and advanced technological developments allow a broader, unspecific analytical approach as either targeted multicomponent analysis or suspect and non-target screening strategies. In order to facilitate such a wide range of compounds, a wide-scope sample clean-up method for high-volume air samples based on a combination of adsorbents was applied, followed by comprehensive two-dimensional gas chromatography separation and low-resolution time-of-flight mass spectrometric detection (GC × GC-LRMS). During the study reported here, simultaneous non-target and suspect screening were applied. The detection of over 700 compounds of interest in the particle phase and over 1200 compounds in the gaseous phase is reported. Of those, 62 compounds were confirmed with reference standards and 90 compounds with a probable structure (based upon mass spectrometric interpretation and library spectrum comparison). These included compounds already detected in Arctic matrices and compounds not detected previously (see also Fig. 1). In addition, 241 compounds were assigned a tentative structure or compound class. Hitherto unknown halogenated compounds, which are not listed in the mass spectral libraries used, were also detected and partly identified.

2020

Quantifying the Impact of the Covid-19 Lockdown Measures on Nitrogen Dioxide Levels throughout Europe

Solberg, Sverre; Walker, Sam-Erik; Schneider, Philipp; Guerreiro, Cristina

In this paper, the effect of the lockdown measures on nitrogen dioxide (NO2) in Europe is analysed by a statistical model approach based on a generalised additive model (GAM). The GAM is designed to find relationships between various meteorological parameters and temporal metrics (day of week, season, etc.) on the one hand and the level of pollutants on the other. The model is first trained on measurement data from almost 2000 monitoring stations during 2015–2019 and then applied to the same stations in 2020, providing predictions of expected concentrations in the absence of a lockdown. The difference between the modelled levels and the actual measurements from 2020 is used to calculate the impact of the lockdown measures adjusted for confounding effects, such as meteorology and temporal trends. The study is focused on April 2020, the month with the strongest reductions in NO2, as well as on the gradual recovery until the end of July. Significant differences between the countries are identified, with the largest NO2 reductions in Spain, France, Italy, Great Britain and Portugal and the smallest in eastern countries (Poland and Hungary). The model is found to perform best for urban and suburban sites. A comparison between the found relative changes in urban surface NO2 data during the lockdown and the corresponding changes in tropospheric vertical NO2 column density as observed by the TROPOMI instrument on Sentinel-5P revealed good agreement despite substantial differences in the observing method.

2021

Review of Interpreting Gaseous Pollution Data Regarding Heritage Objects

Thickett, David; Grøntoft, Terje

Pollutant gases pose a significant risk to some cultural heritage objects, and surveys have shown that the professionals involved consider themselves to lack knowledge to fully assess risk. Three approaches towards risk assessment, research results, standards and damage functions have been considered. An assessment tool has been developed, collating over 4000 research reports into a scheme for the impact on 22 materials of acetic and formic acids, nitrogen dioxide, ozone and reduced sulphur gases. The application of doses or concentrations has been considered, the impact of measurement time compared to annual exposure investigated and a simple tool derived.

2023

Organochlorines, perfluoroalkyl substances, mercury, and egg incubation temperature in an Arctic seabird: Insights from data loggers

Blévin, Pierre; Shaffer, Scott A.; Bustamante, Paco; Angelier, Frédéric; Picard, Baptiste; Herzke, Dorte; Moe, Børge; Gabrielsen, Geir W.; Bustnes, Jan Ove; Chastel, Olivier

In birds, incubation‐related behaviors and brood patch formation are influenced by hormonal regulation such as prolactin secretion. Brood patch provides efficient heat transfer between the incubating parent and the developing embryo in the egg. Importantly, several environmental contaminants are already known to have adverse effects on avian reproduction. However, relatively little is known about the effect of contaminants on incubation temperature (Tinc) in wild birds. By using temperature thermistors placed into artificial eggs, we investigated whether the most contaminated parent birds are less able to provide appropriate egg warming and thus less committed to incubating their clutch. Specifically, we investigated the relationships among 3 groups of contaminants (organochlorines, perfluoroalkyl substances [PFASs], and mercury [Hg]) with Tinc and also with prolactin concentrations and brood patch size in incubating Arctic black‐legged kittiwakes (Rissa tridactyla). Our results reveal that among the organochlorines considered, only blood levels of oxychlordane, the main metabolite of chlordane, a banned pesticide, were negatively related to the minimum incubation temperature in male kittiwakes. Levels of PFASs and Hg were unrelated to Tinc in kittiwakes. Moreover, our study suggests a possible underlying mechanism: since we reported a significant and negative association between blood oxychlordane concentrations and the size of the brood patch in males. Finally, this reduced Tinc in the most oxychlordane‐contaminated kittiwakes was associated with a lower egg hatching probability.

2018

Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling

Tichý, Ondřej; Eckhardt, Sabine; Balkanski, Yves; Hauglustaine, Didier; Evangeliou, Nikolaos

Ammonia (NH3), a significant precursor of particulate matter, affects not only biodiversity, ecosystems, and soil acidification but also climate and human health. In addition, its concentrations are constantly rising due to increasing feeding needs and the large use of fertilization and animal farming. Despite the significance of ammonia, its emissions are associated with large uncertainties, while its atmospheric abundance is difficult to measure. Nowadays, satellite products can effectively measure ammonia with low uncertainty and a global coverage. Here, we use satellite observations of column ammonia in combination with an inversion algorithm to derive ammonia emissions with a high resolution over Europe for the period 2013–2020. Ammonia emissions peak in northern Europe due to agricultural application and livestock management, in western Europe (industrial activity), and over Spain (pig farming). Emissions have decreased by −26 % since 2013 (from 5431 Gg in 2013 to 3994 Gg in 2020), showing that the abatement strategies adopted by the European Union have been very efficient. The slight increase (+4.4 %) in 2015 is also reproduced here and is attributed to some European countries exceeding annual emission targets. Ammonia emissions are low in winter (286 Gg) and peak in summer (563 Gg) and are dominated by the temperature-dependent volatilization of ammonia from the soil. The largest emission decreases were observed in central and eastern Europe (−38 %) and in western Europe (−37 %), while smaller decreases were recorded in northern (−17 %) and southern Europe (−7.6 %). When complemented with ground observations, modelled concentrations using the posterior emissions showed improved statistics, also following the observed seasonal trends. The posterior emissions presented here also agree well with respective estimates reported in the literature and inferred from bottom-up and top-down methodologies. These results indicate that satellite measurements combined with inverse algorithms constitute a robust tool for emission estimates and can infer the evolution of ammonia emissions over large timescales.

2023

Combined Contaminant Levels from Local Harvested Food Items in the Norwegian–Finnish–Russian Border Region

Nalbandyan-Schwarz, Anna; Pedersen, Kristine Bondo; Evenset, Anita; Heimstad, Eldbjørg Sofie; Sandanger, Torkjel Manning; Myllynen, Päivi; Rautio, Arja

This paper presents the results of a multidisciplinary study with the aim of assessing the potential combined risk from consuming locally harvested food products in the Euro-Arctic region of Norway, Finland, and Russia. The three important contaminant groups—radioactive substances, heavy metals, and persistent organic pollutants (POPs)—were measured in food samples such as berries, mushrooms, fish, birds, reindeer, and moose; they were sampled in 2013–2015. To assess the combined pollution levels and investigate the trends, similarities, and variations between different contaminant groups, subsequent multivariate statistical analysis was performed. The results showed that, in general, the levels of radioactive substances, toxic elements, and POPs were below the permitted EU maximum content in food products. However, statistical analysis revealed some correlations, similarities, and peculiarities between the accumulation of different contaminants in various species, which allowed for a better understanding of the mechanisms of accumulation and interaction between different contaminant groups. It also gave a better insight into the possible added risks and helped pinpoint species that could serve as reference markers for the accumulation of different contaminants in food. Mushrooms, fish, and reindeer were found to be important markers in the combined risk assessments for the contents of metals and radioactive substances. Further research, as well as the development of methodologies for combined assessments, are recommended.

2024

Sb-PiPLU: A Novel Parametric Activation Function for Deep Learning

Mondal, Ayan; Shrivastava, Vimal K.; Chatterjee, Ayan; Ramachandra, Raghavendra

The choice of activation function—particularly non-linear ones—plays a vital role in enhancing the classification performance of deep neural networks. In recent years, a variety of non-linear activation functions have been proposed. However, many of these suffer from drawbacks that limit the effectiveness of deep learning models. Common issues include the dying neuron problem, bias shift, gradient explosion, and vanishing gradients. To address these challenges, we introduce a new activation function: Softsign-based Piecewise Parametric Linear Unit (Sb-PiPLU). This function offers improved non-linear approximation capabilities for neural networks. Its piecewise, parametric design allows for greater adaptability and flexibility, which in turn enhances overall model performance. We evaluated Sb-PiPLU through a series of image classification experiments across various Convolutional Neural Network (CNN) architectures. Additionally, we assessed its memory usage and computational cost, demonstrating that Sb-PiPLU is both stable and efficient in practical applications. Our experimental results show that Sb-PiPLU consistently outperforms conventional activation functions in both classification accuracy and computational efficiency. It achieved higher accuracy on multiple benchmark datasets, including CIFAR-10, CINIC-10, MWD, Brain Tumor, and SVHN, surpassing widely-used functions such as ReLU and Tanh. Due to its flexibility and robustness, Sb-PiPLU is particularly well-suited for complex image classification tasks.

2025

Seasonal and latitudinal variability in the atmospheric concentrations of cyclic volatile methyl siloxanes in the Northern Hemisphere

Wania, Frank; Warner, Nicholas Alexander; McLachlan, Michael S; Durham, Jeremy; Lei, Ying Duan; Xu, Shihe

Field data from two latitudinal transects in Europe and Canada were gathered to better characterize the atmospheric fate of three cyclic methylsiloxanes (cVMSs), i.e., octamethyl-cyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6). During a year-long, seasonally resolved outdoor air sampling campaign, passive samplers with an ultra-clean sorbent were deployed at 15 sampling sites covering latitudes ranging from the source regions (43.7–50.7 °N) to the Arctic (79–82.5 °N). For each site, one of two passive samplers and one of two field blanks were separately extracted and analyzed for the cVMSs at two different laboratories using gas-chromatography-mass spectrometry. Whereas the use of a particular batch of sorbent and the applied cleaning procedure to a large extent controlled the levels of cVMS in field blanks, and therefore also the method detection and quantification limits, minor site-specific differences in field blank contamination were apparent. Excellent agreement between duplicates was obtained, with 95% of the concentrations reported by the two laboratories falling within a factor of 1.6 of each other. Nearly all data show a monotonic relationship between the concentration and distance from the major source regions. Concentrations in source regions were comparatively constant throughout the year, while the concentration gradient towards remote regions became steeper during summer when removal via OH radicals is at its maximum. Concentrations of the different cVMS oligomers were highly correlated within a given transect. Changes in relative abundance of cVMS oligomers along the transect were in agreement with relative atmospheric degradation rates via OH radicals.

2023

Trends, composition, and sources of carbonaceous aerosol at the Birkenes Observatory, northern Europe, 2001–2018

Yttri, Karl Espen; Canonaco, Francesco; Eckhardt, Sabine; Evangeliou, Nikolaos; Fiebig, Markus; Gundersen, Hans; Hjellbrekke, Anne-Gunn; Myhre, Cathrine Lund; Platt, Stephen Matthew; Prévôt, André S. H.; Simpson, David; Solberg, Sverre; Surratt, Jason D.; Tørseth, Kjetil; Uggerud, Hilde Thelle; Vadset, Marit; Wan, Xin; Aas, Wenche

We present 18 years (2001–2018) of aerosol measurements, including organic and elemental carbon (OC andEC), organic tracers (levoglucosan, arabitol, mannitol, trehalose, glucose, and 2-methyltetrols), trace elements, andions, at the Birkenes Observatory (southern Norway) – a site representative of the northern European region. The OC/EC (2001–2018) and the levoglucosan (2008–2018) time series are the longest in Europe, with OC/EC available for the PM10, PM2.5 (fine), and PM10–2.5 (coarse) size fractions, providing the opportunity for a nearly 2-decade-long assessment. Using positive matrix factorization (PMF), we identify seven carbonaceous aerosol sources at Birkenes: mineral-dust-dominated aerosol (MIN), traffic/industry-like aerosol (TRA/IND), short-range-transported biogenic secondary organic aerosol (BSOASRT), primary biological aerosol particles (PBAP), biomass burning aerosol (BB), ammonium-nitrate-dominated aerosol (NH4NO3), and (one low carbon fraction) sea salt aerosol (SS).
We observed significant (p < 0.05), large decreases in EC in PM10 (−3.9 % yr−1) and PM2.5 (−4.2 % yr−1) anda smaller decline in levoglucosan (−2.8 % yr−1), suggesting that OC/EC from traffic and industry is decreasing, whereas the abatement of OC/EC from biomass burning has beenslightly less successful. EC abatement with respect to anthropogenic sources is further supported by decreasing EC fractions in PM2.5 (−3.9 % yr−1) and PM10(−4.5 % yr−1).
PMF apportioned 72 % of EC to fossil fuel sources; this was further supported by PMF applied to absorption photometer data, which yielded a two-factor solution with alow aerosol Ångstrøm exponent (AAE=0.93) fraction, as-sumed to be equivalent black carbon from fossil fuel combustion (eBCFF), contributing 78 % to eBC mass. The higher AAE fraction (AAE=2.04) is likely eBC from BB (eBCBB). Source–receptor model calculations (FLEXPART) showed that continental Europe and western Russia were the main source regions of both elevated eBCBB and eBCFF.
Dominating biogenic sources explain why there was no downward trend for OC. A relative increase in the OC fraction in PM2.5(+3.2 % yr−1) and PM10(+2.4 % yr−1) underscores the importance of biogenic sources at Birkene (BSOA and PBAP), which were higher in the vegetative season and dominated both fine (53 %) and coarse (78 %) OC. Furthermore, 77 %–91 % of OC in PM2.5, PM10–2.5, and PM10 was attributed to biogenic sources in summer vs. 22 %–37 % in winter. The coarse fraction had the highest share of biogenic sources regardless of season and was dominated by PBAP, except in winter. Our results show a shift in the aerosol composition at Birkenes and, thus, also in the relative source contributions. The need for diverse offline and online carbonaceous aerosol speciation to understand carbonaceous aerosol sources, including their seasonal, annual, and long-term variability, has been demonstrated.

2021

Development of a supramolecular solvent–based extraction method for application to quantitative analyses of a wide range of organic contaminants in indoor dust

Marcinekova, Paula; Melymuk, Lisa; Bohlin-Nizzetto, Pernilla; Martinelli, Erika; Jilkova, Simona Rozárka; Martiník, Jakub; Senk, Petr; Kukučka, Petr; Audyc, Ondřej; Kohoutek, Jiří; Ghebremeskel, Mebrat; Håland, Alexander; Borgen, Anders; Eikenes, Heidi; Hanssen, Linda; Harju, Mikael; Cebula, Zofia; Rostkowski, Pawel

This study investigates the efficacy of supramolecular solvent (SUPRAS) in extracting a diverse spectrum of organic contaminants from indoor dust. Initially, seven distinct SUPRAS were assessed across nine categories of contaminants to identify the most effective one. A SUPRAS comprising Milli-Q water, tetrahydrofuran, and hexanol in a 70:20:10 ratio, respectively, demonstrated the best extraction performance and was employed for testing a wider array of organic contaminants. Furthermore, we applied the selected SUPRAS for the extraction of organic compounds from the NIST Standard Reference Material (SRM) 2585. In parallel, we performed the extraction of NIST SRM 2585 with conventional extraction methods using hexane:acetone (1:1) for non-polar contaminants and methanol (100%) extraction for polar contaminants. Analysis from two independent laboratories (in Norway and the Czech Republic) demonstrated the viability of SUPRAS for the simultaneous extraction of twelve groups of organic contaminants with a broad range of physico-chemical properties including plastic additives, pesticides, and combustion by-products. However, caution is advised when employing SUPRAS for highly polar contaminants like current-use pesticides or volatile substances like naphthalene.

2024

Snow buntings (Plectrophenax nivealis) as bio-indicators for exposure differences to legacy and emerging persistent organic pollutants from the Arctic terrestrial environment on Svalbard

Warner, Nicholas Alexander; Sagerup, Kjetil; Kristoffersen, Siv; Herzke, Dorte; Gabrielsen, Geir W.; Jenssen, Bjørn Munro

Eggs of snow buntings (Plectrophenax nivealis) were applied as a bio-indicator to examine differences in exposure to legacy persistent organic pollutants (POPs) and perflouroalkyl subtances (PFAS) from the terrestrial environment surrounding the settlements of Longyearbyen, Barentsburg and Pyramiden on Svalbard, Norway. Significantly higher concentrations of summed polychlorinated biphenyls (sumPCB7) in eggs collected from Barentsburg (2980 ng/g lipid weight (lw)) and Pyramiden (3860 ng/g lw) compared to Longyearbyen (96 ng/g lw) are attributed to local sources of PCBs within these settlements. Similar findings were observed for p,p′-dichlorodiphenyldichloroethylene (p,p′-DDE) where higher median concentrations observed in Pyramiden (173 ng/g lw) and Barentsburg (75 ng/g lw) compared to Longyearbyen (48 ng/g lw) may be influenced by guano inputs from breeding seabird populations, although other point sources cannot be ruled out. Concentrations of perfluorooctane sulphonate (PFOS) and several perfluorinated carboxylic acids (PFCAs) in snow bunting eggs were found to be statistically higher in the populated settlements of Longyearbyen and Barentsburg compared to the abandoned Pyramiden. Narrow foraging ranges of snow buntings during breeding season was useful in assessing point sources of exposure for PCBs and PFAS at particular sites with extreme differences observed between nest locations. SumPCB7 concentrations ranged from 2 μg/g ww to below detection limits between nest sites located less than a kilometer from each other in Pyramiden. Similar findings were observed in Longyearbyen, where several PFCAs ranged from 2 to 55 times higher between nest sites with similar spatial distances. These findings indicate that snow buntings can be a useful bio-indicator offering high spatial resolution for contaminant source apportionment in terrestrial environments on Svalbard.

2019

Modeling the Influence of Eutrophication and Redox Conditions on Mercury Cycling at the Sediment-Water Interface in the Berre Lagoon

Pakhomova, Svetlana; Yakushev, Evgeniy; Protsenko, Elizaveta; Rigaud, Sylvain; Cossa, Daniel; Knoery, Joel; Couture, Raoul-Marie; Radakovitch, Olivier; Yakubov, Shamil; Krzeminska, Dominika; Newton, Alice

This study presents a specifically designed Mercury module in a coupled benthic-pelagic reactive-transport model - Bottom RedOx Model (BROM) that allows to study mercury (Hg) biogeochemistry under different conditions. This module considers the transformation of elemental mercury (Hg(0)), divalent mercury (Hg(II)) and methylmercury (MeHg). The behavior of mercury species in the model is interconnected with changes of oxygen, hydrogen sulfide, iron oxides, organic matter, and biota. We simulated the transformation and transport of Hg species in the water column and upper sediment layer under five different scenarios, combining various levels of oxygenation and trophic state in the Berre lagoon, a shallow eutrophic lagoon of the French Mediterranean coast subjected to seasonal anoxia. The first scenario represents the conditions in the lagoon that are compared with experimental data. The four other scenarios were produced by varying the biological productivity, using low and high nutrient (N and P) concentrations, and by varying the redox conditions using different intensity of vertical mixing in the water column. The results of the simulation show that both oxidized and reduced sediments can accumulate Hg, but any shifts in redox conditions in bottom water and upper sediment layer lead to the release of Hg species into the water column. Eutrophication and/or restricted vertical mixing lead to reducing conditions and intensify MeHg formation in the sediment with periodic release to the water column. Oxygenation of an anoxic water body can lead to the appearance of Hg species in the water column and uptake by organisms, whereby Hg may enter into the food web. The comparison of studied scenarios shows that a well-oxygenated eutrophic system favors the conditions for Hg species bioaccumulation with a potential adverse effect on the ecosystem. The research is relevant to the UN Minimata convention, EU policies on water, environmental quality standards and Mercury in particular.

2018

Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe

Ge, Yao; Solberg, Sverre; Heal, Mathew R; Reimann, Stefan; Caspel, Willem van; Hellack, Bryan; Salameh, Therese; Simpson, David

Atmospheric volatile organic compounds (VOCs) constitute a wide range of species, acting as precursors to ozone and aerosol formation. Atmospheric chemistry and transport models (CTMs) are crucial to understanding the emissions, distribution, and impacts of VOCs. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West (EMEP MSC-W) CTM to evaluate emission inventories in Europe. Here we undertake the first intensive model–measurement comparison of VOCs in 2 decades. The modelled surface concentrations are evaluated both spatially and temporally, using measurements from the regular EMEP monitoring network in 2018 and 2019, as well as a 2022 campaign. To achieve this, we utilised the UK National Atmospheric Emissions Inventory to derive explicit emission profiles for individual species and employed a tracer method to produce pure concentrations that are directly comparable to observations.

The degree to which the modelled and measured VOCs agree varies depending on the specific species. The model successfully captures the overall spatial and temporal variations of major alkanes (e.g. ethane, n-butane) and unsaturated species (e.g. ethene, benzene) but less so for propane, i-butane, and ethyne. This discrepancy underscores potential issues in the boundary conditions for the latter species and in their primary emissions from, in particular, the solvent and road transport sectors. Specifically, potential missing propane emissions and issues with its boundary conditions are highlighted by large model underestimations and smaller propane-to-ethane ratios compared to the measurement. Meanwhile, both the model and measurements show strong linear correlations among butane isomers and among pentane isomers, indicating common sources for these pairs of isomers. However, modelled ratios of i-butane to n-butane and i-pentane to n-pentane are approximately one-third of the measured ratios, which is largely driven by significant emissions of n-butane and n-pentane from the solvent sector. This suggests issues with the speciation profile of the solvent sector, underrepresented contributions from transport and fuel evaporation sectors in current inventories, or both. Furthermore, the modelled ethene-to-ethyne and benzene-to-ethyne ratios differ significantly from measured ratios. The different model performance strongly points to shortcomings in the spatial and temporal patterns and magnitudes of ethyne emissions, especially during winter. For OVOCs, the modelled and measured concentrations of methanal and methylglyoxal show a good agreement, despite a moderate underestimation by the model in summer. This discrepancy could be attributed to an underestimation of contributions from biogenic sources or possibly a model overestimation of their photolytic loss in summer. However, the insufficiency of suitable measurements limits the evaluation of other OVOCs. Finally, model simulations employing the CAMS inventory show slightly better agreements with measurements than those using the Centre on Emission Inventories and Projections (CEIP) inventory. This enhancement is likely due to the CAMS inventory's detailed segmentation of the road transport sector, including its associated sub-sector-specific emission profiles. Given this improvement, alongside the previously mentioned concerns about the model's biased estimations of various VOC ratios, future efforts should focus on a more detailed breakdown of dominant emission sectors (e.g. solvents) and the refinement of their speciation profiles to improve model accuracy.

2024

Understanding the role of cities and citizen science in advancing sustainable development goals across Europe: insights from European research framework projects

Liu, Hai Ying; Ahmed, Sohel; Passani, Antonella; Bartonova, Alena

This paper examines the potential impact of citizen science on achieving SDGs in cities. The analysis focuses on projects funded through the European Research Framework Programmes that utilize citizen science practices to involve cities and citizens in addressing sustainability issues. We analyzed a total of 44 projects active between 2016 and 2027, encompassing both ongoing and completed projects. Instead of relying solely on existing literature, we utilized a project database called CORDIS to gather project information. This approach allowed us to develop a comprehensive framework by utilizing uniformly classified data from the database, which is not typically available in literature. Using a four-stage framework analysis method, we assessed the projects' thematic areas, goals, types of solution promoted or tested to address sustainability challenges, methodologies employed, and the impacts achieved or expected. Through this analysis, we identified successful collaborations between citizen science and cities, showcasing examples of effective practice where citizens and cities co-created and tested solutions that contribute to SDGs. This highlights the active role that citizens, as participants or citizen scientists, play in the transition toward SDGs. This study focuses on more than 100 European cities that have been involved in EU-funded research projects implementing and planning to conduct citizen science activities, which directly and indirectly link to various SDGs. Our findings reveal that citizen science practices in cities predominantly address SDG3 (Good health and wellbeing), 11 (Sustainable cities and communities), and 13 (Climate action). Cities that engage citizens in co-creating solutions can enhance their capacity to improve quality of life and reduce climate and environmental impacts. Citizen engagement at the city and community levels can bolster efforts toward achieving SDGs and monitoring progress on a city-wide scale. However, to fully integrate citizen science and its contribution to cities in achieving SDGs, further research is needed to align the SDGs formulated at the national level with those at the city level. This entails exploring how citizen science can align with SDGs indicators and the quantification of SDG targets. Such efforts will facilitate the mainstreaming of citizen science and its potential to drive progress toward SDGs in cities.

2023

Estimation of the historical dry deposition of air pollution indoors to the monumental paintings by Edvard Munch in the University Aula, in Oslo, Norway

Grøntoft, Terje; Frøysaker, Tine

The historical (1835–2020) deposition of major air pollutants (SO2, NOx, O3 and PM2.5) indoors, as represented by the monumental Edvard Munch paintings (c. 220 m2) installed in 1916 in the Oslo University Aula in Norway, were approximated from the outdoor air concentrations, indoor to outdoor concentration ratios and dry deposition velocities. The annual deposition of the pollutants to the paintings was found to have been 4–25 times lower than has been reported to buildings outdoors in the urban background in the centre of Oslo. It reflected the outdoor deposition but varied less, from 0.3 to 1.2 g m−2 a−1. The accumulated deposition since 1916, and then not considering the regularly performed cleaning of the paintings, was found to have been 43 ± 13 g m−2, and 110 ± 40 g m−2 in a similar situation since 1835. The ozone deposition, and the PM2.5 deposition before the 1960s, were a relatively larger part of the accumulated total indoor (to the paintings) than reported outdoor deposition. About 18 and 33 times more O3 than NOx and PM2.5 deposition was estimated to the paintings in 2020, as compared to the about similar reported outdoor dry deposition of O3 and NOx. The deposition of PM2.5 to the paintings was probably reduced with about 62% (50–80%) after installation of mechanical filtration in 1975 and was estimated to be 0.011 (± 0.006) g m−2 in 2020.

2022

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