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Whereas inhalation exposure to organic contaminants can negatively impact human health, knowledge of their spatial variability in the ambient atmosphere remains limited. We analyzed the extracts of passive air samplers deployed at 119 unique sites in Southern Canada between 2019 and 2022 for 353 organic vapors. Hierarchical clustering of the obtained data set revealed four archetypes of spatial concentration variability in the outdoor atmosphere, which are indicative of common sources and similar atmospheric dispersion behavior. “Point Source” signatures are characterized by elevated concentration in the vicinity of major release locations. A “Population” signature applies to compounds whose air concentrations are highly correlated with population density, and is associated with emissions from consumer products. The “Water Source” signature applies to substances with elevated levels in the vicinity of water bodies from which they evaporate. Another group of compounds displays a “Uniform” signature, indicative of a lack of major sources within the study area. We illustrate how such a data set, and the derived spatial patterns, can be applied to support the identification of sources, the quantification of atmospheric emissions, the modeling of air quality, and the investigation of potential inequities in inhalation exposure.
2024
2018
In support of the global stocktake of the Paris Agreement on climate change, this study presents a comprehensive framework to process the results of an ensemble of atmospheric inversions in order to make their net ecosystem exchange (NEE) carbon dioxide (CO2) flux suitable for evaluating national greenhouse gas inventories (NGHGIs) submitted by countries to the United Nations Framework Convention on Climate Change (UNFCCC). From inversions we also deduced anthropogenic methane (CH4) emissions regrouped into fossil and agriculture and waste emissions, as well as anthropogenic nitrous oxide (N2O) emissions. To compare inversion results with national reports, we compiled a new global harmonized database of emissions and removals from periodical UNFCCC inventories by Annex I countries, and from sporadic and less detailed emissions reports by non-Annex I countries, given by national communications and biennial update reports. No gap filling was applied. The method to reconcile inversions with inventories is applied to selected large countries covering ∼90 % of the global land carbon uptake for CO2 and top emitters of CH4 and N2O. Our method uses results from an ensemble of global inversions produced by the Global Carbon Project for the three greenhouse gases, with ancillary data. We examine the role of CO2 fluxes caused by lateral transfer processes from rivers and from trade in crop and wood products and the role of carbon uptake in unmanaged lands, both not accounted for by NGHGIs. Here we show that, despite a large spread across the inversions, the median of available inversion models points to a larger terrestrial carbon sink than inventories over temperate countries or groups of countries of the Northern Hemisphere like Russia, Canada and the European Union. For CH4, we find good consistency between the inversions assimilating only data from the global in situ network and those using satellite CH4 retrievals and a tendency for inversions to diagnose higher CH4 emission estimates than reported by NGHGIs. In particular, oil- and gas-extracting countries in central Asia and the Persian Gulf region tend to systematically report lower emissions compared to those estimated by inversions. For N2O, inversions tend to produce higher anthropogenic emissions than inventories for tropical countries, even when attempting to consider only managed land emissions. In the inventories of many non-Annex I countries, this can be tentatively attributed to a lack of reporting indirect N2O emissions from atmospheric deposition and from leaching to rivers, to the existence of natural sources intertwined with managed lands, or to an underestimation of N2O emission factors for direct agricultural soil emissions. Inversions provide insights into seasonal and interannual greenhouse gas fluxes anomalies, e.g., during extreme events such as drought or abnormal fire episodes, whereas inventory methods are established to estimate trends and multi-annual changes. As a much denser sampling of atmospheric CO2 and CH4 concentrations by different satellites coordinated into a global constellation is expected in the coming years, the methodology proposed here to compare inversion results with inventory reports (e.g., NGHGIs) could be applied regularly for monitoring the effectiveness of mitigation policy and progress by countries to meet the objective of their pledges. The dataset constructed by this study is publicly available at https://doi.org/10.5281/zenodo.5089799 (Deng et al., 2021).
2022
This paper presents a modelling study on the fate of CHBr3 and its product gases in the troposphere within the context of tropical deep convection. A cloud-scale case study was conducted along the west coast of Borneo, where several deep convective systems were triggered on the afternoon and early evening of 19 November 2011. These systems were sampled by the Falcon aircraft during the field campaign of the SHIVA project and analysed using a simulation with the cloud-resolving meteorological model C-CATT-BRAMS at 2×2 km resolution that represents the emissions, transport by large-scale flow, convection, photochemistry, and washout of CHBr3 and its product gases (PGs). We find that simulated CHBr3 mixing ratios and the observed values in the boundary layer and the outflow of the convective systems agree. However, the model underestimates the background CHBr3 mixing ratios in the upper troposphere, which suggests a missing source at the regional scale. An analysis of the simulated chemical speciation of bromine within and around each simulated convective system during the mature convective stage reveals that >85 % of the bromine derived from CHBr3 and its PGs is transported vertically to the point of convective detrainment in the form of CHBr3 and that the remaining small fraction is in the form of organic PGs, principally insoluble brominated carbonyls produced from the photo-oxidation of CHBr3. The model simulates that within the boundary layer and free troposphere, the inorganic PGs are only present in soluble forms, i.e. HBr, HOBr, and BrONO2, and, consequently, within the convective clouds, the inorganic PGs are almost entirely removed by wet scavenging. We find that HBr is the most abundant PG in background lower-tropospheric air and that this prevalence of HBr is a result of the relatively low background tropospheric ozone levels at the regional scale. Contrary to a previous study in a different environment, for the conditions in the simulation, the insoluble Br2 species is hardly formed within the convective systems and therefore plays no significant role in the vertical transport of bromine. This likely results from the relatively small quantities of simulated inorganic bromine involved, the presence of HBr in large excess compared to HOBr and BrO, and the relatively efficient removal of soluble compounds within the convective column.
2021
Modeling study of the impact of SO2 volcanic passive emissions on the tropospheric sulfur budget
Well constrained volcanic emissions inventories in chemistry transport models are necessary to study the impacts induced by these sources on the tropospheric sulfur composition and on sulfur species concentrations and depositions at the surface. In this paper, the changes induced by the update of the volcanic sulfur emissions inventory are studied using the global chemistry transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Échelle). Unlike the previous inventory (Andres and Kasgnoc, 1998), the updated one (Carn et al., 2016, 2017) uses more accurate information and includes contributions from both passive degassing and eruptive emissions. Eruptions are provided as daily total amounts of sulfur dioxide (SO2) emitted by volcanoes in the Carn et al. (2016, 2017) inventories, and degassing emissions are provided as annual averages with the related mean annual uncertainties of those emissions by volcano. Information on plume altitudes is also available and has been used in the model. We chose to analyze the year 2013, for which only a negligible amount of eruptive volcanic SO2 emissions is reported, allowing us to focus the study on the impact of passive degassing emissions on the tropospheric sulfur budget. An evaluation against the Ozone Monitoring Instrument (OMI) SO2 total column and MODIS (Moderate-Resolution Imaging Spectroradiometer) aerosol optical depth (AOD) observations shows the improvements of the model results with the updated inventory. Because the global volcanic SO2 flux changes from 13 Tg yr−1 in Andres and Kasgnoc (1998) to 23.6 Tg yr−1 in Carn et al. (2016, 2017), significant differences appear in the global sulfur budget, mainly in the free troposphere and in the tropics. Even though volcanic SO2 emissions represent 15 % of the total annual sulfur emissions, the volcanic contribution to the tropospheric sulfate aerosol burden is 25 %, which is due to the higher altitude of emissions from volcanoes. Moreover, a sensitivity study on passive degassing emissions, using the annual uncertainties of emissions per volcano, also confirmed the nonlinear link between tropospheric sulfur species content with respect to volcanic SO2 emissions. This study highlights the need for accurate estimates of volcanic sources in chemistry transport models in order to properly simulate tropospheric sulfur species.
2021
The increased availability of commercially-available low-cost air quality sensors combined with increased interest in their use by citizen scientists, community groups, and professionals is resulting in rapid adoption, despite data quality concerns. We have characterized three out-the-box PM sensor systems under different environmental conditions, using field colocation against reference equipment. The sensor systems integrate Plantower 5003, Sensirion SPS30 and Alphasense OCP-N3 PM sensors. The first two use photometry as a measuring technique, while the third one is an optical particle counter. For the performance evaluation, we co-located 3 units of each manufacturer and compared the results against optical (FIDAS) and gravimetric (KFG) methods for a period of 7 weeks (28 August to 19 October 2020). During the period from 2nd and 5th October, unusually high PM concentrations were observed due to a long-range transport episode. The results show that the highest correlations between the sensor systems and the optical reference are observed for PM1, with coefficients of determination above 0.9, followed by PM2.5. All the sensor units struggle to correctly measure PM10, and the coefficients of determination vary between 0.45 and 0.64. This behavior is also corroborated when using the gravimetric method, where correlations are significantly higher for PM2.5 than for PM10, especially for the sensor systems based on photometry. During the long range transport event the performance of the photometric sensors was heavily affected, and PM10 was largely underestimated. The sensor systems evaluated in this study had good agreement with the reference instrumentation for PM1 and PM2.5; however, they struggled to correctly measure PM10. The sensors also showed a decrease in accuracy when the ambient size distribution was different from the one for which the manufacturer had calibrated the sensor, and during weather conditions with high relative humidity. When interpreting and communicating air quality data measured using low-cost sensor systems, it is important to consider such limitations in order not to risk misinterpretation of the resulting data.
2021
2019
Can plastic related chemicals be indicators of plastic ingestion in an Arctic seabird?
For decades, the northern fulmar (Fulmarus glacialis) has been found to ingest and accumulate high loads of plastic due to its feeding ecology and digestive tract morphology. Plastic ingestion can lead to both physical and toxicological effects as ingested plastics can be a pathway for hazardous chemicals into seabirds' tissues. Many of these contaminants are ubiquitous in the environment and the contribution of plastic ingestion to the uptake of those contaminants in seabirds’ tissues is poorly known. In this study we aimed at quantifying several plastic-related chemicals (PRCs) -PBDE209, several dechloranes and several phthalate metabolites- and assessing their relationship with plastic burdens (both mass and number) to further investigate their potential use as proxies for plastic ingestion. Blood samples from fulmar fledglings and liver samples from both fledgling and non-fledgling fulmars were collected for PRC quantification. PBDE209 and dechloranes were quantified in 39 and 33 livers, respectively while phthalates were quantified in plasma. Plastic ingestion in these birds has been investigated previously and showed a higher prevalence in fledglings. PBDE209 was detected in 28.2 % of the liver samples. Dechlorane 602 was detected in all samples while Dechloranes 601 and 604 were not detected in any sample. Dechlorane 603 was detected in 11 individuals (33%). Phthalates were detected in one third of the analysed blood samples. Overall, no significant positive correlation was found between plastic burdens and PRC concentrations. However, a significant positive relationship between PBDE209 and plastic number was found in fledglings, although likely driven by one outlier. Our study shows the complexity of PRC exposure, the timeline of plastic ingestion and subsequent uptake of PRCs into the tissues in birds, the additional exposure of these chemicals via their prey, even in a species ingesting high loads of plastic.
2024
Concentration Fluctuations from Localized Atmospheric Releases
We review the efforts made by the scientific community in more than seventy years to elucidate the behaviour of concentration fluctuations arising from localized atmospheric releases of dynamically passive and non-reactive scalars. Concentration fluctuations are relevant in many fields including the evaluation of toxicity, flammability, and odour nuisance. Characterizing concentration fluctuations requires not just the mean concentration but also at least the variance of the concentration in the location of interest. However, for most purposes the characterization of the concentration fluctuations requires knowledge of the concentration probability density function (PDF) in the point of interest and even the time evolution of the concentration. We firstly review the experimental works made both in the field and in the laboratory, and cover both point sources and line sources. Regarding modelling approaches, we cover analytical, semi-analytical, and numerical methods. For clarity of presentation we subdivide the models in two groups, models linked to a transport equation, which usually require a numerical resolution, and models mainly based on phenomenological aspects of dispersion, often providing analytical or semi-analytical relations. The former group includes: large-eddy simulations, Reynolds-averaged Navier–Stokes methods, two-particle Lagrangian stochastic models, PDF transport equation methods, and heuristic Lagrangian single-particle methods. The latter group includes: fluctuating plume models, semi-empirical models for the concentration moments, analytical models for the concentration PDF, and concentration time-series models. We close the review with a brief discussion highlighting possible useful additions to experiments and improvements to models.
2020
Sheath formation time for spherical Langmuir probes
The formation time of the surrounding sheath of Langmuir probes in an ionospheric plasma has been studied to better understand the constraints this puts on the sampling frequency of a probe. A fully kinetic three-dimensional particle-in-cell model is used to simulate the temporal effects in the electron saturation region as the sheath forms. The stability of the probe current and the stability of the ion and electron density in the vicinity of the probe have been used to evaluate when the sheath was formed. Simulated results were compared with theoretical models and are in good agreement with the theoretical results. This shows that theoretical models can be used as guidance to estimate the formation time and to determine the sampling rate for a swept bias Langmuir system. Our results also show that the formation time is less affected by the plasma temperature and bias voltage as we move into the thick sheath regime, and will instead be determined by the plasma density. The presented results also show that applying a step function to the probe could be used to characterise ions species composition, or to estimate the ion density.
2023
Based upon the thermodynamic simulation of a biogas-SOFC integrated process and the costing of its elements, the present work examines the economic feasibility of biogas-SOFCs for combined heat and power (CHP) generation, by the comparison of their economic performance against the conventional biogas-CHP with internal combustion engines (ICEs), under the same assumptions. As well as the issues of process scale and an SOFC’s cost, examined in the literature, the study brings up the determinative effects of: (i) the employed SOFC size, with respect to its operational point, as well as (ii) the feasibility criterion, on the feasibility assessment. Two plant capacities were examined (250 m3·h−1 and 750 m3·h−1 biogas production), and their feasibilities were assessed by the Internal Rate of Return (IRR), the Net Present Value (NPV) and the Pay Back Time (PBT) criteria. For SOFC costs at 1100 and 2000 EUR·kWel−1, foreseen in 2035 and 2030, respectively, SOFCs were found to increase investment (by 2.5–4.5 times, depending upon a plant’s capacity and the SOFC’s size) and power generation (by 13–57%, depending upon the SOFC’s size), the latter increasing revenues. SOFC-CHP exhibits considerably lower IRRs (5.3–13.4% for the small and 16.8–25.3% for the larger plant), compared to ICE-CHP (34.4%). Nonetheless, according to NPV that does not evaluate profitability as a return on investment, small scale biogas-SOFCs (NPVmax: EUR 3.07 M) can compete with biogas-ICE (NPV: EUR 3.42 M), for SOFCs sized to operate at 70% of the maximum power density (MPD) and with a SOFC cost of 1100 EUR·kWel−1, whereas for larger plants, SOFC-CHP can lead to considerably higher NPVs (EUR 12.5–21.0 M) compared to biogas-ICE (EUR 9.3 M). Nonetheless, PBTs are higher for SOFC-CHP (7.7–11.1 yr and 4.2–5.7 yr for the small and the large plant, respectively, compared to 2.3 yr and 3.1 yr for biogas-ICE) because the criterion suppresses the effect of SOFC-CHP-increased revenues to a time period shorter than the plant’s lifetime. Finally, the economics of SOFC-CHP are optimized for SOFCs sized to operate at 70–82.5% of their MPD, depending upon the SOFC cost and the feasibility criterion. Overall, the choice of the feasibility criterion and the size of the employed SOFC can drastically affect the economic evaluation of SOFC-CHP, whereas the feasibility criterion also determines the economically optimum size of the employed SOFC.
2022
Total oxidizable precursors assay for PFAS in human serum
Per- and polyfluoroalkyl substances (PFAS) are a class of chemicals including over 4700 substances. As a limited number of PFAS is routinely analyzed in human serum, complementary analytical methods are required to characterize the overlooked fraction. A promising tool is the total oxidizable precursors (TOP) assay to look for precursors by oxidation to perfluoroalkyl acids (PFAA). The TOP assay was originally developed for large volumes of water and had to be adapted for 250 μL of human serum. Optimization of the method was performed on serum samples spiked with model precursors. Oxidative conditions similar to previous TOP assay methods were not sufficient for complete oxidation of model precursors. Prolonged heating time (24 h) and higher oxidant amount (95 mg of Na2S2O8 per 225 μL of serum) were needed for complete conversion of the model precursors and accomplishing PFAA yields of 35–100 %. As some precursors are not fully converted to PFAA, the TOP assay can only provide semi-quantitative estimates of oxidizable precursors in human serum. However, the TOP assay can be used to give indications about the identity of unknown precursors by evaluating the oxidation products, including perfluoroalkyl sulfonic acids (PFSA) and perfluoroalkyl ether carboxylic acids (PFECA). The optimized TOP assay for human serum opens the possibility for high-throughput screening of human serum for undetected PFAA precursors.
2022
Environmental contaminants are found throughout Arctic marine ecosystems, and their presence in seabirds has been
associated with toxicological responses. However, there are few studies of genotoxicity in Arctic avian wildlife. The purpose of
the present study was to quantify deoxyribonucleic acid (DNA) damage in lymphocytes of selected seabird species and to
examine whether accumulation of organohalogen contaminants (SOHCs) affects DNA damage. Blood was sampled from
common eider (Somateria mollissima), black guillemot (Cepphus grylle), black-legged kittiwake (Rissa tridactyla), glaucous gull
(Larus hyperboreus), arctic skua (Stercorarius parasiticus), and great skua (Stercorarius skua) in Kongsfjorden, Svalbard (Norway).
Contaminant concentrations found in the 6 species differed, presumably because of foraging ecology and biomagnification.
Despite large differences in contaminant concentrations, ranging from SOHCs 3.3 ng/g wet weight in the common eider to
SOHCs 895 ng/g wet weight in the great skua, there was no strong difference among the species in baseline DNA damage or
sensitivity to a genotoxic stressor (hydrogen peroxide). Baseline levels of DNA damage were low, with median values ranging
from 1.7% in the common eider to 8.6% in the great skua. There were no associations between DNA damage and contaminants
in the investigated species, suggesting that contaminant concentrations in Kongsfjorden are too low to evoke genotoxic effects,
or possibly that lymphocytes are resistant to strand breakage. Clearly, genotoxicity is a topic for future studies of Arctic seabirds
Arctic; Seabirds; Genotoxicity; Comet Assay; Persistent organic pollutants; Perfluoroalkyl substances
2018
Deployment and Evaluation of a Network of Open Low-Cost Air Quality Sensor Systems
Low-cost air quality sensors have the potential to complement the regulatory network of air quality monitoring stations, with respect to increased spatial density of observations, however, their data quality continues to be of concern. Here we report on our experience with a small network of open low-cost sensor systems for air quality, which was deployed in the region of Stavanger, Norway, under Nordic winter conditions. The network consisted of AirSensEUR sensor systems, equipped with sensors for, among others, nitrogen dioxide and fine particulate matter. The systems were co-located at an air quality monitoring station, for a period of approximately six weeks. A subset of the systems was subsequently deployed at various roadside locations for half a year, and finally co-located at the same air quality monitoring station again, for a post-deployment evaluation. For fine particulate matter, the co-location results indicate a good inter-unit consistency, but poor average out-of-the-box performance (R2 = 0.25, RMSE = 9.6 μ
g m−3). While Köhler correction did not significantly improve the accuracy in our study, filtering for high relative humidity conditions improved the results (R2 = 0.63, RMSE = 7.09 μg m−3). For nitrogen dioxide, the inter-unit consistency was found to be excellent, and calibration models were developed which showed good performance during the testing period (on average R2 = 0.98, RMSE = 5.73 μg m−3), however, due to the short training period, the calibration models are likely not able to capture the full annual variability in environmental conditions. A post-deployment co-location showed, respectively, a slight and significant decrease in inter-sensor consistency for fine particulate matter and nitrogen dioxide. We further demonstrate, how observations from even such a small network can be exploited by assimilation in a high-resolution air quality model, thus adding value to both the observations and the model, and ultimately providing a more comprehensive perspective of air quality than is possible from either of the two input datasets alone. Our study provides valuable insights on the operation and performance of an open sensor system for air quality, particularly under challenging Nordic environmental conditions.
2023
Solar UV radiation measurements in Marambio, Antarctica, during years 2017–2019
In March 2017, measurements of downward global irradiance of ultraviolet (UV) radiation were started with a multichannel GUV-2511 radiometer in Marambio, Antarctica (64.23∘ S; 56.62∘ W), by the Finnish Meteorological Institute (FMI) in collaboration with the Servicio Meteorológico Nacional (SMN). These measurements were analysed and the results were compared to previous measurements performed at the same site with the radiometer of the Antarctic NILU-UV network during 2000–2008 and to data from five stations across Antarctica. In 2017/2018 the monthly-average erythemal daily doses from October to January were lower than those averaged over 2000–2008 with differences from 2.3 % to 25.5 %. In 2017/2018 the average daily erythemal dose from September to March was 1.88 kJ m−2, while in 2018/2019 it was 23 % larger (2.37 kJ m−2). Also at several other stations in Antarctica the UV radiation levels in 2017/2018 were below average. The maximum UV indices (UVI) in Marambio were 6.2 and 9.5 in 2017/2018 and 2018/2019, respectively, whereas during years 2000–2008 the maximum was 12. Cloud cover, the strength of the polar vortex and the stratospheric ozone depletion are the primary factors that influence the surface UV radiation levels in Marambio. The lower UV irradiance values in 2017/2018 are explained by the high ozone concentrations in November, February and for a large part of October. The role of cloud cover was clearly seen in December, and to a lesser extent in October and November, when cloud cover qualitatively explains changes which could not be ascribed to changes in total ozone column (TOC). In this study, the roles of aerosols and albedo are of minor influence because the variation of these factors in Marambio was small from one year to the other. The largest variations of UV irradiance occur during spring and early summer when noon solar zenith angle (SZA) is low and the stratospheric ozone concentration is at a minimum (the so-called ozone hole). In 2017/2018, coincident low total ozone column and low cloudiness near solar noon did not occur, and no extreme UV indices were measured.
2020
Global predictions of primary soil salinization under changing climate in the 21st century
Soil salinization has become one of the major environmental and socioeconomic issues globally and this is expected to be exacerbated further with projected climatic change. Determining how climate change influences the dynamics of naturally-occurring soil salinization has scarcely been addressed due to highly complex processes influencing salinization. This paper sets out to address this long-standing challenge by developing data-driven models capable of predicting primary (naturally-occurring) soil salinity and its variations in the world’s drylands up to the year 2100 under changing climate. Analysis of the future predictions made here identifies the dryland areas of South America, southern and western Australia, Mexico, southwest United States, and South Africa as the salinization hotspots. Conversely, we project a decrease in the soil salinity of the drylands in the northwest United States, the Horn of Africa, Eastern Europe, Turkmenistan, and west Kazakhstan in response to climate change over the same period.
2021
2022
2019
In the framework of the RECCAP2 initiative, we present the greenhouse gas (GHG) and carbon (C) budget of Europe. For the decade of the 2010s, we present a bottom-up (BU) estimate of GHG net-emissions of 3.9 Pg CO2-eq. yr−1 (using a global warming potential on a 100 years horizon), which are largely dominated by fossil fuel emissions. In this decade, terrestrial ecosystems acted as a net GHG sink of 0.9 Pg CO2-eq. yr−1, dominated by a CO2 sink that was partially counterbalanced by net emissions of CH4 and N2O. For CH4 and N2O, we find good agreement between BU and top-down (TD) estimates from atmospheric inversions. However, our BU land CO2 sink is significantly higher than the TD estimates. We further show that decadal averages of GHG net-emissions have declined by 1.2 Pg CO2-eq. yr−1 since the 1990s, mainly due to a reduction in fossil fuel emissions. In addition, based on both data driven BU and TD estimates, we also find that the land CO2 sink has weakened over the past two decades. A large part of the European CO2 and C sinks is located in Northern Europe. At the same time, we find a decreasing trend in sink strength in Scandinavia, which can be attributed to an increase in forest management intensity. These are partly offset by increasing CO2 sinks in parts of Eastern Europe and Northern Spain, attributed in part to land use change. Extensive regions of high CH4 and N2O emissions are mainly attributed to agricultural activities and are found in Belgium, the Netherlands and the southern UK. We further analyzed interannual variability in the GHG budgets. The drought year of 2003 shows the highest net-emissions of CO2 and of all GHGs combined.
2024
The Sentinel-5 Precursor (S5P) satellite operated by the European Space Agency has carried the TROPOspheric Monitoring Instrument (TROPOMI) on a Sun-synchronous low-Earth orbit since 13 October 2017. The S5P mission has acquired more than 5 years of TROPOMI nadir ozone profile data retrieved from the level 0 to 1B processor version 2.0 and the level 1B to 2 optimal-estimation-based processor version 2.4.0. The latter is described in detail in this work, followed by the geophysical validation of the resulting ozone profiles for the period May 2018 to April 2023. Comparison of TROPOMI ozone profile data to co-located ozonesonde and lidar measurements used as references concludes to a median agreement better than 5 % to 10 % in the troposphere. The bias goes up to −15 % in the upper stratosphere (35–45 km) where it can exhibit vertical oscillations. The comparisons show a dispersion of about 30 % in the troposphere and 10 % to 20 % in the upper troposphere to lower stratosphere and in the middle stratosphere, which is close to mission requirements. Chi-square tests of the observed differences confirm on average the validity of the ex ante (prognostic) satellite and ground-based data uncertainty estimates in the middle stratosphere above about 20 km. Around the tropopause and below, the mean chi-square value increases up to about four, meaning that the ex ante TROPOMI uncertainty is underestimated. The information content of the ozone profile retrieval is characterised by about five to six vertical subcolumns of independent information and a vertical sensitivity (i.e. the fraction of the information that originates from the measurement) nearly equal to unity at altitudes from about 20 to 50 km, decreasing rapidly at altitudes above and below. The barycentre of the retrieved information is usually close to the nominal retrieval altitude in the 20–50 km altitude range, with positive and negative offsets of up to 10 km below and above this range, respectively. The effective vertical resolution of the profile retrieval usually ranges within 10–15 km, with a minimum close to 7 km in the middle stratosphere. Increased sensitivities and higher effective vertical resolutions are observed at higher solar zenith angles (above about 60°), as can be expected, and correlate with higher retrieved ozone concentrations. The vertical sensitivity of the TROPOMI tropospheric ozone retrieval is found to depend on the solar zenith angle, which translates into a seasonal and meridian dependence of the bias with respect to reference measurements. A similar although smaller effect can be seen for the viewing zenith angle. Additionally, the bias is negatively correlated with the surface albedo for the lowest three ozone subcolumns (0–18 km), despite the albedo's apparently slightly positive correlation with the retrieval degrees of freedom in the signal. For the 5 years of TROPOMI ozone profile data that are available now, an overall positive drift is detected for the same three subcolumns, while a negative drift is observed above (24–32 km), resulting in a negligible vertically integrated drift.
2024
The participation of a diverse –in terms of geography, discipline and gender– group of Early Career Researchers (ECRs) in the peer review process can help alleviate the workload of senior researchers and counteract the perceptual biases that the latter tend to show. Moreover, ECRs can benefit from developing skills that are often not included in educational programs. From 2018 to 2021, the Association of Polar Early Career Scientists, in collaboration with other associations, organized six group reviews of the Intergovernmental Panel on Climate Change (IPCC) reports by a total of more than 600 ECRs from over 70 different countries. This study aims to evaluate this group review in terms of its contribution to the production of scientific knowledge, and as a career development opportunity for ECRs. The data analyzed consists of application forms, review comments, and feedback surveys that were collected during each review process. The results of this study show that, overall, the group reviews were a success in terms of the experience of ECRs and their contribution to the peer review of the IPCC reports. Most survey respondents considered the general organization of the group reviews satisfactory and expressed interest in participating in future group reviews. However, most participants did not engage in discussions with their peers, which constitutes a missed opportunity to engage in active learning and the shared production of knowledge. ECRs made a significant contribution to the review of the IPCC reports by producing an average of 2,422 ± 532 comments per group review, 36% of which were substantive. PhD students were shown to be as proficient reviewers as postdoctoral researchers and faculty reviewers. More importantly, the diversity of reviewers in terms of geography and discipline, together with the fact that they are ECRs, can help produce more balanced scientific reports since they bring new perspectives, thus counteracting the biases that senior researchers have. These group reviews could be improved by providing more comprehensive training and facilitating communication among reviewers so that they can engage in meaningful exchanges. We conclude that the IPCC should formalize the inclusion of ECRs in future reviews of the IPCC reports.
2024
Comparison of particle number size distribution trends in ground measurements and climate models
Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.
2022
Electronic waste (e-waste) is informally processed and recycled in Agbogbloshie in Accra (Ghana), which may be the largest such site in West Africa. This industry can lead to significant environmental contamination. In this study, surface dust samples were collected at a range of sites within Accra to establish the offsite consequences of such activities. Fifty-one samples were collected and analysed for 69 elements by ICP-mass spectrometry after nitric acid digestion. The data indicated a significant enrichment in metals associated with solder and copper wire at the site itself and a downwind dispersion of this source material to a distance of approximately 2.0 km. Chlorine and bromine were also elevated at this site as residues from polyvinyl chloride combustion and flame retardants respectively. The elemental composition indicated that only low technology electrical equipment was being treated this way. Multivariate statistical analyses by principal components analysis and polytopic vector analysis identified three sources contributing to the system; (i) burn site residue dispersing within 2 km from the source site, (ii) marine matter on the beaches alone and (iii) the baseline soil conditions of the city of Accra. Risk ratios and hazard quotients developed from the measured concentrations indicated that copper was providing the greatest risk to inhabitants in most cases although nickel, vanadium, chromium and zinc also contributed.
2019
2019