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Microfluidic In Vitro Platform for (Nano)Safety and (Nano)Drug Efficiency Screening
Microfluidic technology is a valuable tool for realizing more in vitro models capturing cellular and organ level responses for rapid and animal‐free risk assessment of new chemicals and drugs. Microfluidic cell‐based devices allow high‐throughput screening and flexible automation while lowering costs and reagent consumption due to their miniaturization. There is a growing need for faster and animal‐free approaches for drug development and safety assessment of chemicals (Registration, Evaluation, Authorisation and Restriction of Chemical Substances, REACH). The work presented describes a microfluidic platform for in vivo‐like in vitro cell cultivation. It is equipped with a wafer‐based silicon chip including integrated electrodes and a microcavity. A proof‐of‐concept using different relevant cell models shows its suitability for label‐free assessment of cytotoxic effects. A miniaturized microscope within each module monitors cell morphology and proliferation. Electrodes integrated in the microfluidic channels allow the noninvasive monitoring of barrier integrity followed by a label‐free assessment of cytotoxic effects. Each microfluidic cell cultivation module can be operated individually or be interconnected in a flexible way. The interconnection of the different modules aims at simulation of the whole‐body exposure and response and can contribute to the replacement of animal testing in risk assessment studies in compliance with the 3Rs to replace, reduce, and refine animal experiments.
2021
Long-term monitoring of regulated organic chemicals, such as legacy persistent organic pollutants (POPs) and polycyclic aromatic hydrocarbons (PAHs), in ambient air provides valuable information about the compounds' environmental fate as well as temporal and spatial trends. This is the foundation to evaluate the effectiveness of national and international regulations for priority pollutants. Extracts of high-volume air samples, collected on glass fibre filters (GFF for particle phase) and polyurethane foam plugs (PUF for gaseous phase), for targeted analyses of legacy POPs are commonly cleaned by treatment with concentrated sulfuric acid, resulting in extracts clean from most interfering compounds and matrices that are suitable for multi-quantitative trace analysis. Such standardised methods, however, severely restrict the number of analytes for quantification and are not applicable when targeting new and emerging compounds as some may be less stable under acid treatment. Recently developed suspect and non-target screening analytical strategies (SUS and NTS, respectively) are shown to be effective evaluation tools aimed at identifying a high number of compounds of emerging concern. These strategies, combining highly sophisticated analytical technology with extensive data interpretation and statistics, are already widely accepted in environmental sciences for investigations of various environmental matrices, but their application to air samples is still very limited. In order to apply SUS and NTS for the identification of organic contaminants in air samples, an adapted and more wide-scope sample clean-up method is needed compared to the traditional method, which uses concentrated sulfuric acid. Analysis of raw air sample extracts without clean-up would generate extensive contamination of the analytical system, especially with PUF matrix-based compounds, and thus highly interfered mass spectra and detection limits which are unacceptable high for trace analysis in air samples.
In this study, a novel wide-scope sample clean-up method for high-volume air samples has been developed and applied to real high-volume air samples, which facilitates simultaneous target, suspect and non-target analyses. The scope and efficiency of the method were quantitatively evaluated with organic compounds covering a wide range of polarities (logP 2–11), including legacy POPs, brominated flame retardants (BFRs), chlorinated pesticides and currently used pesticides (CUPs). In addition, data reduction and selection strategies for SUS and NTS were developed for comprehensive two-dimensional gas chromatography separation with low-resolution time-of-flight mass spectrometric detection (GC × GC-LRMS) data and applied to real high-volume air samples. Combination of the newly developed clean-up procedure and data treatment strategy enabled the prioritisation of over 600 compounds of interest in the particle phase (on GFF) and over 850 compounds in the gas phase (on PUF) out of over 25 000 chemical features detected in the raw dataset. Of these, 50 individual compounds were identified and confirmed with reference standards, 80 compounds were identified with a probable structure, and 774 compounds were assigned to various compound classes. In the dataset available here, 11 hitherto unknown halogenated compounds were detected. These unknown compounds were not yet listed in the available mass spectral libraries.
2021
2021
Low concentrations of 106Ru were detected across Europe at the turn of September and October 2017. The origin of 106Ru has still not been confirmed; however, current studies agree that the release occurred probably near Mayak in the southern Urals. The source reconstructions are mostly based on an analysis of concentration measurements coupled with an atmospheric transport model. Since reasonable temporal resolution of concentration measurements is crucial for proper source term reconstruction, the standard 1-week sampling interval could be limiting. In this paper, we present an investigation of the usability of the newly developed AMARA (Autonomous Monitor of Atmospheric Radioactive Aerosol) and CEGAM (carousel gamma spectrometry) real-time monitoring systems, which are based on the gamma-ray counting of aerosol filters and allow for determining the moment when 106Ru arrived at the monitoring site within approx. 1 h and detecting activity concentrations as low as several mBq m−3 in 4 h intervals. These high-resolution data were used for inverse modeling of the 106Ru release. We perform backward runs of the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) atmospheric transport model driven with meteorological data from the Global Forecast System (GFS), and we construct a source–receptor sensitivity (SRS) matrix for each grid cell of our domain. Then, we use our least squares with adaptive prior covariance (LS-APC) method to estimate possible locations of the release and the source term of the release. With Czech monitoring data, the use of concentration measurements from the standard regime and from the real-time regime is compared, and a better source reconstruction for the real-time data is demonstrated in the sense of the location of the source and also the temporal resolution of the source. The estimated release location, Mayak, and the total estimated source term, 237±107 TBq, are in agreement with previous studies. Finally, the results based on the Czech monitoring data are validated with the IAEA-reported (International Atomic Energy Agency) dataset with a much better spatial resolution, and the agreement between the IAEA dataset and our reconstruction is demonstrated. In addition, we validated our findings also using the FLEXPART (FLEXible PARTicle dispersion) model coupled with meteorological analyses from the European Centre for Medium-Range Weather Forecasts (ECMWF).
2021
Instead of a flag valid/non-valid usually proposed in the quality control (QC) processes of air quality (AQ), we proposed a method that predicts the p-value of each observation as a value between 0 and 1. We based our error predictions on three approaches: the one proposed by the Working Group on Guidance for the Demonstration of Equivalence (European Commission (2010)), the one proposed by Wager (Journal of Machine Learning Research, 15, 1625–1651 (2014)) and the one proposed by Lu (Journal of Machine Learning Research, 22, 1–41 (2021)). Total Error framework enables to differentiate the different errors: input, output, structural modeling and remnant. We thus theoretically described a one-site AQ prediction based on a multi-site network using Random Forest for regression in a Total Error framework. We demonstrated the methodology with a dataset of hourly nitrogen dioxide measured by a network of monitoring stations located in Oslo, Norway and implemented the error predictions for the three approaches. The results indicate that a simple one-site AQ prediction based on a multi-site network using Random Forest for regression provides moderate metrics for fixed stations. According to the diagnostic based on predictive qq-plot and among the three approaches used in this study, the approach proposed by Lu provides better error predictions. Furthermore, ensuring a high precision of the error prediction requires efforts on getting accurate input, output and prediction model and limiting our lack of knowledge about the “true” AQ phenomena. We put effort in quantifying each type of error involved in the error prediction to assess the error prediction model and further improving it in terms of performance and precision.
2021
2021
A comprehensive European dataset on monthly atmospheric NH3, acid gases (HNO3, SO2, HCl), and aerosols (NH+4, NO−3, SO2−4, Cl−, Na+, Ca2+, Mg2+) is presented and analysed. Speciated measurements were made with a low-volume denuder and filter pack method (DEnuder for Long-Term Atmospheric sampling, DELTA®) as part of the EU NitroEurope (NEU) integrated project. Altogether, there were 64 sites in 20 countries (2006–2010), coordinated between seven European laboratories. Bulk wet-deposition measurements were carried out at 16 co-located sites (2008–2010). Inter-comparisons of chemical analysis and DELTA® measurements allowed an assessment of comparability between laboratories.
The form and concentrations of the different gas and aerosol components measured varied between individual sites and grouped sites according to country, European regions, and four main ecosystem types (crops, grassland, forests, and semi-natural). The smallest concentrations (with the exception of SO2−4 and Na+) were in northern Europe (Scandinavia), with broad elevations of all components across other regions. SO2 concentrations were highest in central and eastern Europe, with larger SO2 emissions, but particulate SO2−4 concentrations were more homogeneous between regions. Gas-phase NH3 was the most abundant single measured component at the majority of sites, with the largest variability in concentrations across the network. The largest concentrations of NH3, NH+4, and NO−3 were at cropland sites in intensively managed agricultural areas (e.g. Borgo Cioffi in Italy), and the smallest were at remote semi-natural and forest sites (e.g. Lompolojänkkä, Finland), highlighting the potential for NH3 to drive the formation of both NH+4 and NO−3 aerosol. In the aerosol phase, NH+4 was highly correlated with both NO−3 and SO2−4, with a near-1:1 relationship between the equivalent concentrations of NH+4 and sum (NO−3+ SO2−4),of which around 60 % was as NH4NO3.
Distinct seasonality was also observed in the data, influenced by changes in emissions, chemical interactions, and the influence of meteorology on partitioning between the main inorganic gases and aerosol species. Springtime maxima in NH3 were attributed to the main period of manure spreading, while the peak in summer and trough in winter were linked to the influence of temperature and rainfall on emissions, deposition, and gas–aerosol-phase equilibrium. Seasonality in SO2 was mainly driven by emissions (combustion), with concentrations peaking in winter, except in southern Europe, where the peak occurred in summer. Particulate SO2−4 showed large peaks in concentrations in summer in southern and eastern Europe, contrasting with much smaller peaks occurring in early spring in other regions. The peaks in particulate SO2−4 coincided with peaks in NH3 concentrations, attributed to the formation of the stable (NH4)2SO4. HNO3 concentrations were more complex, related to traffic and industrial emissions, photochemistry, and HNO3:NH4NO3 partitioning. While HNO3 concentrations were seen to peak in the summer in eastern and southern Europe (increased photochemistry), the absence of a spring peak in HNO3 in all regions may be explained by the depletion of HNO3 through reaction with surplus NH3 to form the semi-volatile aerosol NH4NO3. Cooler, wetter conditions in early spring favour the formation and persistence of NH4NO3 in the aerosol phase, consistent with the higher springtime concentrations of NH+4 and NO−3. The seasonal profile of NO−3 was mirrored by NH+4, illustrating the influence of gas–aerosol partitioning of NH4NO3 in the seasonality of these components.
Gas-phase NH3 and aerosol NH4NO3 were the dominant species in the total inorganic gas and aerosol species measured in the NEU network. With the current and projected trends in SO2, NOx, and NH3 emissions, concentrations of NH3 and NH4NO3 can be expected to continue to dominate...
2021
Unexpected nascent atmospheric emissions of three ozone-depleting hydrochlorofluorocarbons
Global and regional atmospheric measurements and modeling can play key roles in discovering and quantifying unexpected nascent emissions of environmentally important substances. We focus here on three hydrochlorofluorocarbons (HCFCs) that are restricted by the Montreal Protocol because of their roles in stratospheric ozone depletion. Based on measurements of archived air samples and on in situ measurements at stations of the Advanced Global Atmospheric Gases Experiment (AGAGE) network, we report global abundances, trends, and regional enhancements for HCFC-132b (CH2ClCClF2), which is newly discovered in the atmosphere, and updated results for HCFC-133a (CH2ClCF3) and HCFC-31 (CH2ClF). No purposeful end-use is known for any of these compounds. We find that HCFC-132b appeared in the atmosphere 20 y ago and that its global emissions increased to 1.1 Gg⋅y−1 by 2019. Regional top-down emission estimates for East Asia, based on high-frequency measurements for 2016–2019, account for ∼95% of the global HCFC-132b emissions and for ∼80% of the global HCFC-133a emissions of 2.3 Gg⋅y−1 during this period. Global emissions of HCFC-31 for the same period are 0.71 Gg⋅y−1. Small European emissions of HCFC-132b and HCFC-133a, found in southeastern France, ceased in early 2017 when a fluorocarbon production facility in that area closed. Although unreported emissive end-uses cannot be ruled out, all three compounds are most likely emitted as intermediate by-products in chemical production pathways. Identification of harmful emissions to the atmosphere at an early stage can guide the effective development of global and regional environmental policy.
2021
Although it has been suggested that plastic may act as a vector for pollutants into the tissue of seabirds, the bioaccumulation of harmful contaminants, such as polybrominated diphenyl ethers (PBDEs), released from ingested plastics is poorly understood. Plastic ingestion by the procellariiform species northern fulmar (Fulmarus glacialis) is well documented. In this study, we measured PBDEs levels in liver tissue of northern fulmars without and with (0.13–0.43 g per individual) stomach plastics. PBDE concentrations in the plastic sampled from the same birds were also quantified. Birds were either found dead on beaches in southern Norway or incidentally caught in longline fisheries in northern Norway. PBDEs were detected in all birds but high concentrations were only found in liver samples from beached birds, peaking at 2900 ng/g lipid weight. We found that body condition was a significant factor explaining the elevated concentration levels in livers of beached birds. BDE209 was found in ingested plastic particles and liver tissue of birds with ingested plastics but was absent in the livers of birds without ingested plastics. This strongly suggests a plastic-derived transfer and accumulation of BDE209 to the tissue of fulmars, levels of which might prove useful as a general indicator of plastic ingestion in seabirds.
2021
Implementing Citizen Science in Primary Schools: Engaging Young Children in Monitoring Air Pollution
Most European cities have air pollution levels that exceed the threshold for human health protection. Children are sensitive to air pollution and thus it is important to ensure they are not exposed to high concentrations of air pollutants. In order to make a positive change toward cleaner air, a joint effort is needed, involving all civil society actors. Schools and local communities have a decisive role, and can, for example, become engaged in citizen science initiatives and knowledge coproduction. In 2019, with the aim of raising awareness for air quality, NILU developed a citizen science toolbox to engage primary schools in monitoring air quality using a simple and affordable measuring method based on paper and petroleum jelly. This is a very visual method, where the students can clearly see differences from polluted and non-polluted places by looking at “how dirty” is the paper. In addition to the qualitative analysis, we have developed an air meter scale making possible for the students to obtain an indicative measurement of the air pollution level. The comparison between the paper and petroleum jelly method against reference PM10 data collected at two official air quality stations showed a good agreement. The method is a strong candidate for dust monitoring in citizen science projects, making participation possible and empowering people with simple tools at hand. The toolbox is targeted at primary schools and children aged 6–12 years, although it can easily be adapted to other age groups. The main objective of the toolbox is to involve young children who are usually not targeted in air quality citizen science activities, to develop research skills and critical thinking, as well as increase their awareness about the air they breathe. The toolbox is designed to engage students in hands-on activities, that challenge them to create hypotheses, design scientific experiments, draw conclusions and find creative solutions to the air pollution problem. The toolbox includes all the necessary material for the teachers, including guidance, background information and templates facilitating the incorporation in the school curricula. The toolbox was launched as part of the Oslo European Green Capital in March 2019 and was later included as part of the European Clean Air Day initiative coordinated by the European Citizen Science Association (ECSA) working group on air quality. A total of 30 schools and 60 4th grade classes (aged 8–9 years) participated in the Oslo campaign. The citizen science approach employed in the schools, combined the four key elements that promote knowledge integration: elicit ideas, add new ideas, distinguish among ideas and reflect and sort out ideas. Although the main goal of the study was to provide simple but robust tools for engaging young children in air quality monitoring, we also carried out ex-ante and ex-post evaluations in 12 of the participating classes using a 10-question multiple choice test to have an indication of the contribution of the activity to knowledge integration. The results show that there is an increase in the number of correct answers, as well as a reduction in the misconceptions after conducting the activity. These results indicate that applying a citizen science approach improved science instruction and helped knowledge integration by including students' views and taking advantage of the diverse ideas students generated. Citizen science gives learners an insight into the ways that scientists generate solutions for societal problems. But more important, citizen science provides a way to differ from the classic view of the learner as an absorber of information, by considering the social context of instruction and making the topic personally relevant.
2021
Quantitative chemical analysis of airborne particulate matter (PM) is vital for the understanding of health effects in indoor and outdoor environments, as well as for enforcing EU air quality regulations. Typically, airborne particles are sampled over long time periods on filters, followed by lab-based analysis, e.g., with inductively coupled plasma mass spectrometry (ICP-MS). During the EURAMET EMPIR AEROMET project, cascade impactor aerosol sampling is combined for the first time with on-site total reflection X-ray fluorescence (TXRF) spectroscopy to develop a tool for quantifying particle element compositions within short time intervals and even on-site. This makes variations of aerosol chemistry observable with time resolution only a few hours and with good size resolution in the PM10 range. The study investigates the proof of principles of this methodological approach. Acrylic discs and silicon wafers are shown to be suitable impactor carriers with sufficiently smooth and clean surfaces, and a non-destructive elemental mass concentration measurement with a lower limit of detection around 10 pg/m3 could be achieved. We demonstrate the traceability of field TXRF measurements to a radiometrically calibrated TXRF reference, and the results from both analytical methods correspond satisfactorily.
2021
This paper presents the validation results of Aerosol Optical Depth (AOD) retrieved from the Spinning Enhanced Visible Infrared Radiometer (SEVIRI) data using the near-real-time algorithm further developed in the frame of the Satellite-based Monitoring Initiative for Regional Air quality (SAMIRA) project. The SEVIRI AOD was compared against multiple data sources: six stations of the Aerosol Robotic Network (AERONET) in Romania and Poland, three stations of the Aerosol Research Network in Poland (Poland–AOD) and Moderate Resolution Imaging Spectroradiometer (MODIS) data overlapping Romania, Czech Republic and Poland. The correlation values between a four-month dataset (June–September 2014) from SEVIRI and the closest temporally available data for both ground-based and satellite products were identified. The comparison of the SEVIRI AOD with the AERONET AOD observations generally shows a good correlation (r = 0.48–0.83). The mean bias is 0.10–0.14 and the root mean square error RMSE is between 0.11 and 0.15 for all six stations cases. For the comparison with Poland–AOD correlation values are 0.55 to 0.71. The mean bias is 0.04–0.13 and RMSE is between 0.10 and 0.14. As for the intercomparison to MODIS AOD, correlations values were generally lower (r = 0.33–0.39). Biases of −0.06 to 0.24 and RMSE of 0.04 to 0.28 were in good agreement with the ground–stations retrievals. The validation of SEVIRI AOD with AERONET results in the best correlations followed by the Poland–AOD network and MODIS retrievals. The average uncertainty estimates are evaluated resulting in most of the AOD values falling above the expected error range. A revised uncertainty estimate is proposed by including the observed bias form the AERONET validation efforts.
2021
Pollutants emitted by industrial processes are deposited across the landscape. Ice core records from mid-latitude glaciers located close to emission sources document the history of local-to-regional pollution since preindustrial times. Such records underpin attribution of pollutants to specific emission sources critical to developing abatement policies. Previous ice core studies from the Alps document the overall magnitude and timing of pollution related to nitrogen and sulfur-derived species, as well as a few metals including lead. Here, we used subannually resolved measurements of vanadium (V) and molybdenum (Mo) in two ice cores from Col du Dome (French Alps), as well as atmospheric transport and deposition modeling, to investigate sources of pollution in the free European troposphere. The noncrustal V and Mo (ncV, ncMo) components were calculated by subtracting the crustal component from the total concentration. These ice core results showed a 32-fold increase in ncV and a 69-fold increase in ncMo from the preindustrial era (pre-1860) to the industrial concentration peaks. Anthropogenic V and Mo emissions in Europe were estimated using emission factors from oil and coal consumption and atmospheric transport and deposition modeling. When comparing ice core data to estimated anthropogenic V and Mo emissions in Europe, V was found to be sourced primarily from oil combustion emissions. Conversely, coal and oil combustion estimated emissions did not agree with the measured ice core Mo concentrations, suggesting that other anthropogenic Mo sources dominated coal-burning emissions, particularly after the 1950s. Noncoal-burning sources of Mo may include metallurgy although emission factors are poorly known.
2021
Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites.
2021
10-year satellite-constrained fluxes of ammonia improve performance of chemistry transport models
In recent years, ammonia emissions have been continuously increasing, being almost 4 times higher than in the 20th century. Although an important species, as its use as a fertilizer sustains human living, ammonia has major consequences for both humans and the environment because of its reactive gas-phase chemistry that makes it easily convertible to particles. Despite its pronounced importance, ammonia emissions are highly uncertain in most emission inventories. However, the great development of satellite remote sensing nowadays provides the opportunity for more targeted research on constraining ammonia emissions. Here, we used satellite measurements to calculate global ammonia emissions over the period 2008–2017. Then, the calculated ammonia emissions were fed to a chemistry transport model, and ammonia concentrations were simulated for the period 2008–2017.
The simulated concentrations of ammonia were compared with ground measurements from Europe, North America and Southeastern Asia, as well as with satellite measurements. The satellite-constrained ammonia emissions represent global concentrations more accurately than state-of-the-art emissions. Calculated fluxes in the North China Plain were seen to be more increased after 2015, which is not due to emission changes but due to changes in sulfate emissions that resulted in less ammonia neutralization and hence in larger atmospheric loads. Emissions over Europe were also twice as much as those in traditional datasets with dominant sources being industrial and agricultural applications. Four hot-spot regions of high ammonia emissions were seen in North America, which are characterized by high agricultural activity, such as animal breeding, animal farms and agricultural practices. South America is dominated by ammonia emissions from biomass burning, which causes a strong seasonality. In Southeastern Asia, ammonia emissions from fertilizer plants in China, Pakistan, India and Indonesia are the most important, while a strong seasonality was observed with a spring and late summer peak due to rice and wheat cultivation. Measurements of ammonia surface concentrations were better reproduced with satellite-constrained emissions, such as measurements from CrIS (Cross-track Infrared Sounder).
2021
This paper reports on consolidated ground-based validation results of the atmospheric NO2 data produced operationally since April 2018 by the TROPOspheric Monitoring Instrument (TROPOMI) on board of the ESA/EU Copernicus Sentinel-5 Precursor (S5P) satellite. Tropospheric, stratospheric, and total NO2 column data from S5P are compared to correlative measurements collected from, respectively, 19 Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS), 26 Network for the Detection of Atmospheric Composition Change (NDACC) Zenith-Scattered-Light DOAS (ZSL-DOAS), and 25 Pandonia Global Network (PGN)/Pandora instruments distributed globally. The validation methodology gives special care to minimizing mismatch errors due to imperfect spatio-temporal co-location of the satellite and correlative data, e.g. by using tailored observation operators to account for differences in smoothing and in sampling of atmospheric structures and variability and photochemical modelling to reduce diurnal cycle effects. Compared to the ground-based measurements, S5P data show, on average, (i) a negative bias for the tropospheric column data, of typically −23 % to −37 % in clean to slightly polluted conditions but reaching values as high as −51 % over highly polluted areas; (ii) a slight negative median difference for the stratospheric column data, of about −0.2 Pmolec cm−2, i.e. approx. −2 % in summer to −15 % in winter; and (iii) a bias ranging from zero to −50 % for the total column data, found to depend on the amplitude of the total NO2 column, with small to slightly positive bias values for columns below 6 Pmolec cm−2 and negative values above. The dispersion between S5P and correlative measurements contains mostly random components, which remain within mission requirements for the stratospheric column data (0.5 Pmolec cm−2) but exceed those for the tropospheric column data (0.7 Pmolec cm−2). While a part of the biases and dispersion may be due to representativeness differences such as different area averaging and measurement times, it is known that errors in the S5P tropospheric columns exist due to shortcomings in the (horizontally coarse) a priori profile representation in the TM5-MP chemical transport model used in the S5P retrieval and, to a lesser extent, to the treatment of cloud effects and aerosols. Although considerable differences (up to 2 Pmolec cm−2 and more) are observed at single ground-pixel level, the near-real-time (NRTI) and offline (OFFL) versions of the S5P NO2 operational data processor provide similar NO2 column values and validation results when globally averaged, with the NRTI values being on average 0.79 % larger than the OFFL values.
2021
The long-term time trends of atmospheric pollutants at eight Arctic monitoring stations are reported. The work was conducted under the Arctic Monitoring and Assessment Programme (AMAP) of the Arctic Council. The monitoring stations were: Alert, Canada; Zeppelin, Svalbard; Stórhöfði, Iceland; Pallas, Finland; Andøya, Norway; Villum Research Station, Greenland; Tiksi and Amderma, Russia. Persistent organic pollutants (POPs) such as α- and γ-hexachlorocyclohexane (HCH), polychlorinated biphenyls (PCBs), α-endosulfan, chlordane, dichlorodiphenyltrichloroethane (DDT) and polybrominated diphenyl ethers (PBDEs) showed declining trends in air at all stations. However, hexachlorobenzene (HCB), one of the initial twelve POPs listed in the Stockholm Convention in 2004, showed either increasing or non-changing trends at the stations. Many POPs demonstrated seasonality but the patterns were not consistent among the chemicals and stations. Some chemicals showed winter minimum and summer maximum concentrations at one station but not another, and vice versa. The ratios of chlordane isomers and DDT species showed that they were aged residues. Time trends of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) were showing decreasing concentrations at Alert, Zeppelin and Andøya. The Chemicals of Emerging Arctic Concern (CEAC) were either showing stable or increasing trends. These include methoxychlor, perfluorohexane sulfonic acid (PFHxS), 6:2 fluorotelomer alcohol, and C9-C11 perfluorocarboxylic acids (PFCAs). We have demonstrated the importance of monitoring CEAC before they are being regulated because model calculations to predict their transport mechanisms and fate cannot be made due to the lack of emission inventories. We should maintain long-term monitoring programmes with consistent data quality in order to evaluate the effectiveness of chemical control efforts taken by countries worldwide.
2021
2021
While occupational inhalation exposure to gaseous elemental mercury (GEM) has decreased in many workplaces as mercury is being removed from most products and processes, it continues to be a concern for those engaged in artisanal and small-scale gold mining or in recycling mercury-containing products. Recently, stationary and personal passive air samplers based on activated carbon sorbents and radial diffusive barriers have been shown to be suitable for measuring GEM concentrations across the range relevant for chronic health effects. Here, we used a combination of stationary and personal passive samplers to characterize the inhalation exposure to GEM of individuals living and working in two Ghanaian gold mining communities and working at a Norwegian e-waste recycling facility. Exposure concentrations ranging from <7 ng m−3 to >500 μg m−3 were observed, with the higher end of the range occurring in one gold mining community. Large differences in the GEM exposure averaged over the length of a workday between individuals can be rationalized by their activity and proximity to mercury sources. In each of the three settings, the measured exposure of the highest exposed individuals exceeded the highest concentration recorded with a stationary sampler, presumably because those individuals were engaged in an activity that generated or involved GEM vapors. High day-to-day variability in exposure for those who participated on more than one day, suggests the need for sampling over multiple days for reliable exposure characterization. Overall, a combination of personal and stationary passive sampling is a cost-effective approach that cannot only provide information on exposure levels relative to regulatory thresholds, but also can identify emission hotspots and therefore guide mitigation measures.
2021
Concerns have been raised as to whether gunshot fumes induce prolonged reduced lung capacity or even cancer due to inhalation. Gunshot fumes from three different types of ammunition calibre 5.56 mm × 45 NATO were investigated. SS109 has a soft lead (Pb) core, while NM255 and NM229 have a harder steel core. Emissions from ammunitions were characterized with respect to particle number- and mass-size, and mass distribution, heavy metal content, and different gases. Lung epithelial cells were exposed to the fumes at the air liquid interface to elucidate cytotoxicity and genotoxicity. Irrespectively of ammunition type, the largest mass fraction of generated particulate matter (PM) had a size between 1 and 3 μm. The highest number of particles generated was in the size range of 30 nm. Fumes from NM255 and NM229 induced cytotoxic effects of which the emission from NM229 induced the highest effect. Fumes from NM229 induced a dose-related increase in DNA-damage. Significant effects were only achieved at the highest exposure level, which led to approximately 40% reduced cell viability after 24 h. The effect probably relates to the mass of emitted particles where the size may be of importance, in addition to emission of Cu and Zn. A complex mixture of chemical substances and PM may increase the toxicity of the fumes and should encourage measures to reduce exposure.
2021
We synthesized N2O emissions over North America using 17 bottom-up (BU) estimates from 1980–2016 and five top-down (TD) estimates from 1998 to 2016. The BU-based total emission shows a slight increase owing to U.S. agriculture, while no consistent trend is shown in TD estimates. During 2007–2016, North American N2O emissions are estimated at 1.7 (1.0–3.0) Tg N yr−1 (BU) and 1.3 (0.9–1.5) Tg N yr−1 (TD). Anthropogenic emissions were twice as large as natural fluxes from soil and water. Direct agricultural and industrial activities accounted for 68% of total anthropogenic emissions, 71% of which was contributed by the U.S. Our estimates of U.S. agricultural emissions are comparable to the EPA greenhouse gas (GHG) inventory, which includes estimates from IPCC tier 1 (emission factor) and tier 3 (process-based modeling) approaches. Conversely, our estimated agricultural emissions for Canada and Mexico are twice as large as the respective national GHG inventories.
2021
Safety assessment of titanium dioxide (E171) as a food additive
The present opinion deals with an updated safety assessment of the food additive titanium dioxide (E 171) based on new relevant scientific evidence considered by the Panel to be reliable, including data obtained with TiO2 nanoparticles (NPs) and data from an extended one-generation reproductive toxicity (EOGRT) study. Less than 50% of constituent particles by number in E 171 have a minimum external dimension < 100 nm. In addition, the Panel noted that constituent particles < 30 nm amounted to less than 1% of particles by number. The Panel therefore considered that studies with TiO2 NPs < 30 nm were of limited relevance to the safety assessment of E 171. The Panel concluded that although gastrointestinal absorption of TiO2 particles is low, they may accumulate in the body. Studies on general and organ toxicity did not indicate adverse effects with either E 171 up to a dose of 1,000 mg/kg body weight (bw) per day or with TiO2 NPs (> 30 nm) up to the highest dose tested of 100 mg/kg bw per day. No effects on reproductive and developmental toxicity were observed up to a dose of 1,000 mg E 171/kg bw per day, the highest dose tested in the EOGRT study. However, observations of potential immunotoxicity and inflammation with E 171 and potential neurotoxicity with TiO2 NPs, together with the potential induction of aberrant crypt foci with E 171, may indicate adverse effects. With respect to genotoxicity, the Panel concluded that TiO2 particles have the potential to induce DNA strand breaks and chromosomal damage, but not gene mutations. No clear correlation was observed between the physico-chemical properties of TiO2 particles and the outcome of either in vitro or in vivo genotoxicity assays. A concern for genotoxicity of TiO2 particles that may be present in E 171 could therefore not be ruled out. Several modes of action for the genotoxicity may operate in parallel and the relative contributions of different molecular mechanisms elicited by TiO2 particles are not known. There was uncertainty as to whether a threshold mode of action could be assumed. In addition, a cut-off value for TiO2 particle size with respect to genotoxicity could not be identified. No appropriately designed study was available to investigate the potential carcinogenic effects of TiO2 NPs. Based on all the evidence available, a concern for genotoxicity could not be ruled out, and given the many uncertainties, the Panel concluded that E 171 can no longer be considered as safe when used as a food additive.
2021
The effective enrichment of perfluoroalkyl acids (PFAAs) in sea spray aerosols (SSA) demonstrated in previous laboratory studies suggests that SSA is a potential source of PFAAs to the atmosphere. In order to investigate the influence of SSA on atmospheric PFAAs in the field, 48 h aerosol samples were collected regularly between 2018 and 2020 at two Norwegian coastal locations, Andøya and Birkenes. Significant correlations (p < 0.05) between the SSA tracer ion, Na+, and PFAA concentrations were observed in the samples from both locations, with Pearson’s correlation coefficients (r) between 0.4–0.8. Such significant correlations indicate SSA to be an important source of atmospheric PFAAs to coastal areas. The correlations in the samples from Andøya were observed for more PFAA species and were generally stronger than in the samples from Birkenes, which is located further away from the coast and closer to urban areas than Andøya. Factors such as the origin of the SSA, the distance of the sampling site to open water, and the presence of other PFAA sources (e.g., volatile precursor compounds) can have influence on the contribution of SSA to PFAA in air at the sampling sites and therefore affect the observed correlations between PFAAs and Na+.
2021
Why is the city's responsibility for its air pollution often underestimated? A focus on PM2.5
While the burden caused by air pollution in urban areas is well documented, the origin of this pollution and therefore the responsibility of the urban areas in generating this pollution are still a subject of scientific discussion. Source apportionment represents a useful technique to quantify the city's responsibility, but the approaches and applications are not harmonized and therefore not comparable, resulting in confusing and sometimes contradicting interpretations. In this work, we analyse how different source apportionment approaches apply to the urban scale and how their building elements and parameters are defined and set. We discuss in particular the options available in terms of indicator, receptor, source, and methodology. We show that different choices for these options lead to very large differences in terms of outcome. For the 150 large EU cities selected in our study, different choices made for the indicator, the receptor, and the source each lead to an average difference of a factor of 2 in terms of city contribution. We also show that temporal- and spatial-averaging processes applied to the air quality indicator, especially when diverging source apportionments are aggregated into a single number, lead to the favouring of strategies that target background sources while occulting actions that would be efficient in the city centre. We stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility, with important implications. Indeed, if cities are seen as a minor actor, plans will target the background as a priority at the expense of potentially effective local actions.
2021
Tackling Data Quality When Using Low-Cost Air Quality Sensors in Citizen Science Projects
Using low-cost air quality sensors (LCS) in citizen science projects opens many possibilities. LCS can provide an opportunity for the citizens to collect and contribute with their own air quality data. However, low data quality is often an issue when using LCS and with it a risk of unrealistic expectations of a higher degree of empowerment than what is possible. If the data quality and intended use of the data is not harmonized, conclusions may be drawn on the wrong basis and data can be rendered unusable. Ensuring high data quality is demanding in terms of labor and resources. The expertise, sensor performance assessment, post-processing, as well as the general workload required will depend strongly on the purpose and intended use of the air quality data. It is therefore a balancing act to ensure that the data quality is high enough for the specific purpose, while minimizing the validation effort. The aim of this perspective paper is to increase awareness of data quality issues and provide strategies to minimizing labor intensity and expenses while maintaining adequate QA/QC for robust applications of LCS in citizen science projects. We believe that air quality measurements performed by citizens can be better utilized with increased awareness about data quality and measurement requirements, in combination with improved metadata collection. Well-documented metadata can not only increase the value and usefulness for the actors collecting the data, but it also the foundation for assessment of potential integration of the data collected by citizens in a broader perspective.
2021