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Using dispersion models at microscale to assess long-term air pollution in urban hot spots: A FAIRMODE joint intercomparison exercise for a case study in Antwerp

Martín, F.; Janssen, S.; Rodrigues, V.; Sousa, J.; Santiago, J.L.; Rivas, E.; Stocker, J.; Jackson, R.; Russo, F.; Villani, M.G.; Tinarelli, G.; Barbero, D.; José, R. San; Pérez-Camanyo, J.L.; Sousa Santos, Gabriela; Bartzis, J.; Sakellaris, I.; Horváth, Z.; Környei, L.; Liszkai, B.; Kovács, A.; Jurado, X.; Reiminger, N.; Thunis, P.; Cuvelier, C.

In the framework of the Forum for Air Quality Modelling in Europe (FAIRMODE), a modelling intercomparison exercise for computing NO2 long-term average concentrations in urban districts with a very high spatial resolution was carried out. This exercise was undertaken for a district of Antwerp (Belgium). Air quality data includes data recorded in air quality monitoring stations and 73 passive samplers deployed during one-month period in 2016. The modelling domain was 800 × 800 m2. Nine modelling teams participated in this exercise providing results from fifteen different modelling applications based on different kinds of model approaches (CFD – Computational Fluid Dynamics-, Lagrangian, Gaussian, and Artificial Intelligence). Some approaches consisted of models running the complete one-month period on an hourly basis, but most others used a scenario approach, which relies on simulations of scenarios representative of wind conditions combined with post-processing to retrieve a one-month average of NO2 concentrations.

The objective of this study is to evaluate what type of modelling system is better suited to get a good estimate of long-term averages in complex urban districts. This is very important for air quality assessment under the European ambient air quality directives. The time evolution of NO2 hourly concentrations during a day of relative high pollution was rather well estimated by all models. Relative to high resolution spatial distribution of one-month NO2 averaged concentrations, Gaussian models were not able to give detailed information, unless they include building data and street-canyon parameterizations. The models that account for complex urban geometries (i.e. CFD, Lagrangian, and AI models) appear to provide better estimates of the spatial distribution of one-month NO2 averages concentrations in the urban canopy. Approaches based on steady CFD-RANS (Reynolds Averaged Navier Stokes) model simulations of meteorological scenarios seem to provide good results with similar quality to those obtained with an unsteady one-month period CFD-RANS simulations.

Elsevier

2024

Hazard assessment of nanomaterials: how to meet the requirements for (next generation) risk assessment

Longhin, Eleonora Marta; Rios Mondragon, Ivan; Mariussen, Espen; Zheng, Congying; Busquets, Marti; Gajewicz Skrętna, Agnieszka; Hofshagen, Ole-Bendik; Bastus, Neus Gómez; Puntes, Victor Franco; Cimpan, Mihaela-Roxana; Shaposhnikov, Sergey; Dusinska, Maria; Rundén-Pran, Elise

Background

Hazard and risk assessment of nanomaterials (NMs) face challenges due to, among others, the numerous existing nanoforms, discordant data and conflicting results found in the literature, and specific challenges in the application of strategies such as grouping and read-across, emphasizing the need for New Approach Methodologies (NAMs) to support Next Generation Risk Assessment (NGRA). Here these challenges are addressed in a study that couples physico-chemical characterization with in vitro investigations and in silico similarity analyses for nine nanoforms, having different chemical composition, sizes, aggregation states and shapes. For cytotoxicity assessment, three methods (Alamar Blue, Colony Forming Efficiency, and Electric Cell-Substrate Impedance Sensing) are applied in a cross-validation approach to support NAMs implementation into NGRA.

Results

The results highlight the role of physico-chemical properties in eliciting biological responses. Uptake studies reveal distinct cellular morphological changes. The cytotoxicity assessment shows varying responses among NMs, consistent among the three methods used, while only one nanoform gave a positive response in the genotoxicity assessment performed by comet assay.

Conclusions

The study highlights the potential of in silico models to effectively identify biologically active nanoforms based on their physico-chemical properties, reinforcing previous knowledge on the relevance of certain properties, such as aspect ratio. The potential of implementing in vitro methods into NGRA is underlined, cross-validating three cytotoxicity assessment methods, and showcasing their strength in terms of sensitivity and suitability for the testing of NMs.

BioMed Central (BMC)

2024

The dynamics of concentration fluctuations within passive scalar plumes in a turbulent neutral boundary layer

Cassiani, Massimo; Ardeshiri, Hamidreza; Pisso, Ignacio; Salizzoni, Pietro; Marro, Massimo; Stohl, Andreas; Stebel, Kerstin; Park, Soon-Young

We investigate the concentration fluctuations of passive scalar plumes emitted from small, localised (point-like) steady sources in a neutrally stratified turbulent boundary layer over a rough wall. The study utilises high-resolution large-eddy simulations for sources of varying sizes and heights. The numerical results, which show good agreement with wind-tunnel studies, are used to estimate statistical indicators of the concentration field, including spectra and moments up to the fourth order. These allow us to elucidate the mechanisms responsible for the production, transport and dissipation of concentration fluctuations, with a focus on the very near field, where the skewness is found to have negative values – an aspect not previously highlighted. The gamma probability density function is confirmed to be a robust model for the one-point concentration at sufficiently large distances from the source. However, for ground-level releases in a well-defined area around the plume centreline, the Gaussian distribution is found to be a better statistical model. As recently demonstrated by laboratory results, for elevated releases, the peak and shape of the pre-multiplied scalar spectra are confirmed to be independent of the crosswind location for a given downwind distance. Using a stochastic model and theoretical arguments, we demonstrate that this is due to the concentration spectra being directly shaped by the transverse and vertical velocity components governing the meandering of the plume. Finally, we investigate the intermittency factor, i.e. the probability of non-zero concentration, and analyse its variability depending on the thresholds adopted for its definition.

Cambridge University Press

2024

Exploring the connection between COVID19, the energy crisis and PM2.5 emissions from residential heating

Lopez-Aparicio, Susana; Grythe, Henrik; Markelj, Miha; Evangeliou, Nikolaos; Walker, Sam-Erik

Geopolitical events have shown to threaten European energy security in 2022. In Norway, accustomed to low energy prices, the southern part saw 4 times higher electricity prices in 2022 than long term average, whereas in the north, energy prices remained stable. This offers an opportunity to examine the effect of price on household energy consumption and PM2.5 emissions from the residential sector. In the south, electricity consumption went down by 10% while in the north it remained unchanged relative to expected values. While the documented correlation between increased electricity prices and reduced consumption is well-established, our study uniquely captures a substantial shift towards wood as an alternative energy source. In the south, wood for heating increased by approximately 40%, effectively replacing half of the electricity saved. This increase happened despite prices being curbed by strong government subsidies on electricity. Faced with higher energy costs in Europe, we simulate a scenario where consumers across Europe look for affordable energy. With gas and electricity prices predicted to remain well above long-term averages until 2030, biomass will be an attractive option. Our study shows how a shift can endanger Europe's Zero-Pollution strategy, and the need for initiatives targeting the reduction of residential biomass heating.

Elsevier

2024

Comprehensive characterization of European house dust contaminants: Concentrations and profiles, geographical variability, and implications for chemical regulation and health risk

Haglund, Peter; Alygizakis, Nikiforos A.; Covaci, Adrian; Melymuk, Lisa; Bohlin-Nizzetto, Pernilla; Rostkowski, Pawel; Albinet, Alexandre; Alirai, Sylvana; Aurich, Dagny; Bieber, Stefan; Ballesteros-Gómez, Ana; Brennan, Amanda; Budzinski, Hélène; Castro, Gabriela; den Ouden, Fatima; Dévier, Marie-Hélène; Dulio, Valeria; Feng, Yong-Lai; Gabriel, Marta; Gallampois, Christine; Garcia-Vara, Manuel; Giovanoulis, Georgios; Harrad, Stuart; Jacobs, Griet; Jobst, Karl J.; Kaserzon, Sarit; Kumirska, Jolanta; Lestremau, Francois; Lambropoulou, Dimitra; Letzel, Thomas; López de Alda, Miren; Nipen, Maja; Oswald, Peter; Poma, Giulia; Přibylová, Petra; Price, Elliott J.; Raffy, Gaëlle; Schulze, Bastian; Schymanski, Emma L.; Senk, Petr; Wei, Si; Slobodnik, Jaroslav; Talavera Andújar, Begoña; Täubel, Martin; Thomaidis, Nikolaos S.; Wang, Thanh; Wang, Xianyu

Elsevier

2024

Daily high-resolution surface PM2.5 estimation over Europe by ML-based downscaling of the CAMS regional forecast

Shetty, Shobitha; Hamer, Paul David; Stebel, Kerstin; Kylling, Arve; Hassani, Amirhossein; Berntsen, Terje Koren; Schneider, Philipp

Fine particulate matter (PM2.5) is a key air quality indicator due to its adverse health impacts. Accurate PM2.5 assessment requires high-resolution (e.g., atleast 1 km) daily data, yet current methods face challenges in balancing accuracy, coverage, and resolution. Chemical transport models such as those from the Copernicus Atmosphere Monitoring Service (CAMS) offer continuous data but their relatively coarse resolution can introduce uncertainties. Here we present a synergistic Machine Learning (ML)-based approach called S-MESH (Satellite and ML-based Estimation of Surface air quality at High resolution) for estimating daily surface PM2.5 over Europe at 1 km spatial resolution and demonstrate its performance for the years 2021 and 2022. The approach enhances and downscales the CAMS regional ensemble 24 h PM2.5 forecast by training a stacked XGBoost model against station observations, effectively integrating satellite-derived data and modeled meteorological variables. Overall, against station observations, S-MESH (mean absolute error (MAE) of 3.54 μg/m3) shows higher accuracy than the CAMS forecast (MAE of 4.18 μg/m3) and is approaching the accuracy of the CAMS regional interim reanalysis (MAE of 3.21 μg/m3), while exhibiting a significantly reduced mean bias (MB of −0.3 μg/m3 vs. −1.5 μg/m3 for the reanalysis). At the same time, S-MESH requires substantially less computational resources and processing time. At concentrations >20 μg/m3, S-MESH outperforms the reanalysis (MB of −7.3 μg/m3 and -10.3 μg/m3 respectively), and reliably captures high pollution events in both space and time. In the eastern study area, where the reanalysis often underestimates, S-MESH better captures high levels of PM2.5 mostly from residential heating. S-MESH effectively tracks day-to-day variability, with a temporal relative absolute error of 5% (reanalysis 10%). Exhibiting good performance at high pollution events coupled with its high spatial resolution and rapid estimation speed, S-MESH can be highly relevant for air quality assessments where both resolution and timeliness are critical.

Elsevier

2024

Air quality and transport behaviour: sensors, field, and survey data from Warsaw, Poland

Hassani, Amirhossein; Nicińska, Anna; Drabicki, Arkadiusz; Zawojska, Ewa; Sousa Santos, Gabriela; Kula, Grzegorz; Grythe, Henrik; Zawieska, Jakub; Jaczewska, Joanna; Rachubik, Joanna; Archanowicz-Kudelska, Katarzyna; Zagorska, Katarzyna; Grzenda, Maciej; Kubecka, Magdalena; Luckner, Marcin; Jakubczyk, Michał; Wolański, Michał; Castell, Nuria; Gora, Paweł; Skedsmo, Pål Wilter; Rożynek, Satia; Horosiewicz, Szymon

The present study describes the data sets produced in Warsaw, Poland with the aim of developing tools and methods for the implementation of human-centred and data-driven solutions to the enhancement of sustainable mobility transition. This study focuses on school commutes and alternatives to private cars for children drop off and pick up from primary schools. The dataset enables the complex analysis of interactions between determinants of transport mode choice, revealed choices, and air quality impact. We draw on four data collection methods, namely, (i) air quality and noise sensors’ measurements, (ii) in-person observations of transport behaviours, (iii) travel diaries, and (iv) social surveys. Moreover, all trip data from travel diaries are complemented with the calculated attributes of alternative travel modes. The data produced in the project can be also combined with publicly available information on air quality, public transport schedules, and traffic flows. The present data sets help to open new venues for interdisciplinary analyses of sustainable mobility transition effectiveness and efficiency.

Springer Nature

2024

European pollen reanalysis, 1980–2022, for alder, birch, and olive

Sofiev, Mikhail; Palamarchuk, Julia; Kouznetsov, Rostislav; Abramidze, Tamuna; Adams-Groom, Beverley; Antunes, Célia M.; Ariño, Arturo; Bastl, Maximillan; Belmonte, Jordina; Berger, Uwe Edwin; Bonini, Maira; Bruffaerts, Nicolas; Buters, Jeroen T.M.; Cariñanos, Paloma; Celenk, Sevcan; Ceriotti, Valentina; Charalampopoulos, Athanasios; Clewlow, Yolanda; Clot, Bernhard; Dahl, Aslog; Damialis, Athanasios; De Linares, Concepción; de Weger, Letty A; Dirr, Lukas; Ekebom, Agneta; Fatahi, Yalda; Fernández González, Maria; Fernández González, Delia; Fernández-Rodríguez, Santiago; Galán, Carmen; Gedda, Björn; Gehrig, Regula; Geller Bernstein, Carmi; Gonzalez Roldan, Nestor; Grewling, Łukasz; Hajkova, Lenka; Hanninen, Risto; Hentges, François; Jantunen, Juha; Kadantsev, Evgeny; Kasprzyk, Idalia; Kloster, Mathilde; Kluska, Katarzyna; Koenders, Mieke; Lafférsová, Janka; Leru, Poliana Mihaela; Lipiec, Agnieszka; Louna-Korteniemi, Maria; Magyar, Donat; Majkowska-Wojciechowska, Barbara; Mäkelä, Mika; Mitrovic, Mirjana; Myszkowska, Dorota; Oliver, Gilles; Östensson, Pia; Pérez-Badia, Rosa; Piotrowska-Weryszko, Krystyna; Prank, Marje; Przedpelska-Wasowicz, Ewa Maria; Pätsi, Sanna; Rodríguez-Rajo, F. Javier; Ramfjord, Hallvard; Rapiejko, Joanna; Rodinkova, Victoria; Rojo, Jesús; Ruiz-Valenzuela, Luis; Rybnicek, Ondrej; Saarto, Annika; Sauliene, Ingrida; Seliger, Andreja Kofol; Severova, Elena; Shalaboda, Valentina; Sikoparija, Branko; Siljamo, Pilvi; Soares, Joana; Sozinova, Olga; Stangel, Andreas; Stjepanović, Barbara; Teinemaa, Erik; Tyuryakov, Svjatoslav; Trigo, M. Mar; Uppstu, Andreas; Vill, Mart; Vira, Julius; Visez, Nicolas; Vitikainen, Tiina; Vokou, Despoina; Weryszko-Chmielewska, Elzbieta; Karppinen, Ari

The dataset presents a 43 year-long reanalysis of pollen seasons for three major allergenic genera of trees in Europe: alder (Alnus), birch (Betula), and olive (Olea). Driven by the meteorological reanalysis ERA5, the atmospheric composition model SILAM predicted the flowering period and calculated the Europe-wide dispersion pattern of pollen for the years 1980–2022. The model applied an extended 4-dimensional variational data assimilation of in-situ observations of aerobiological networks in 34 European countries to reproduce the inter-annual variability and trends of pollen production and distribution. The control variable of the assimilation procedure was the total pollen release during each flowering season, implemented as an annual correction factor to the mean pollen production. The dataset was designed as an input to studies on climate-induced and anthropogenically driven changes in the European vegetation, biodiversity monitoring, bioaerosol modelling and assessment, as well as, in combination with intra-seasonal observations, for health-related applications.

Springer Nature

2024

Sources and Seasonal Variations of Per- and Polyfluoroalkyl Substances (PFAS) in Surface Snow in the Arctic

Hartz, William Frederik; Björnsdotter, Maria; Yeung, Leo W. Y.; Humby, Jack D.; Eckhardt, Sabine; Evangeliou, Nikolaos; Ericson Jogsten, Ingrid; Kärrman, Anna; Kallenborn, Roland

Per- and polyfluoroalkyl substances (PFAS) are persistent anthropogenic contaminants, some of which are toxic and bioaccumulative. Perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkyl sulfonic acids (PFSAs) can form during the atmospheric degradation of precursors such as fluorotelomer alcohols (FTOHs), N-alkylated perfluoroalkane sulfonamides (FASAs), and hydrofluorocarbons (HFCs). Since PFCAs and PFSAs will readily undergo wet deposition, snow and ice cores are useful for studying PFAS in the Arctic atmosphere. In this study, 36 PFAS were detected in surface snow around the Arctic island of Spitsbergen during January–August 2019 (i.e., 24 h darkness to 24 h daylight), indicating widespread and chemically diverse contamination, including at remote high elevation sites. Local sources meant some PFAS had concentrations in snow up to 54 times higher in Longyearbyen, compared to remote locations. At a remote high elevation ice cap, where PFAS input was from long-range atmospheric processes, the median deposition fluxes of C2–C11 PFCAs, PFOS and HFPO–DA (GenX) were 7.6–71 times higher during 24 h daylight. These PFAS all positively correlated with solar flux. Together this suggests seasonal light is important to enable photochemistry for their atmospheric formation and subsequent deposition in the Arctic. This study provides the first evidence for the possible atmospheric formation of PFOS and GenX from precursors.

2024

A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021

Vojta, Martin; Plach, Andreas; Annadate, Saurabh; Park, Sunyoung; Lee, Gawon; Purohit, Pallav; Lindl, Florian; Lan, Xin; Mühle, Jens; Thompson, Rona Louise; Stohl, Andreas

We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of −0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period.

2024

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