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Atmospheric histories and emissions of chlorofluorocarbons CFC-13 (CClF3), ΣCFC-114 (C2Cl2F4), and CFC-115 (C2ClF5)

Vollmer, Martin K.; Young, Dickon; Trudinger, Cathy M.; Muhle, Jens; Henne, Stephan; Rigby, Matthew; Park, Sunyoung; Li, Shanlan; Guillevic, Myriam; Mitrevski, Blagoj; Harth, Christina M.; Miller, Benjamin R.; Reimann, Stefan; Yao, Bo; Steele, L. Paul; Wyss, Simon A.; Lunder, Chris Rene; Arduini, Jgor; McCulloch, Archie; Wu, Songhao; Rhee, Tae Siek; Wang, Ray H. J.; Salameh, Peter K.; Hermansen, Ove; Hill, Matthias; Langenfelds, Ray L.; Ivy, Diane; O'Doherty, Simon; Krummel, Paul B.; Maione, Michela; Etheridge, David M.; Zhou, Lingxi; Fraser, Paul J.; Prinn, Ronald G.; Weiss, Ray F.; Simmonds, Peter G.

Based on observations of the chlorofluorocarbons CFC-13 (chlorotrifluoromethane), ΣCFC-114 (combined measurement of both isomers of dichlorotetrafluoroethane), and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly 8 decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry-air mole fraction in parts per trillion, pmol mol−1) in 2016. Its growth rate has decreased since the mid-1980s but has remained at a surprisingly high mean level of 0.02 ppt yr−1 since 2000, resulting in a continuing growth of CFC-13 in the atmosphere. ΣCFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.49 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unchanging lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (> 15 % of past peak emissions), of ΣCFC-114 at 1.90 ± 0.84 kt yr−1 (∼ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2015–2016 are 1.14 ± 0.50 kt yr−1 and have doubled compared to the 2007–2010 minimum. We find CFC-13 emissions from aluminum smelters but if extrapolated to global emissions, they cannot account for the lingering global emissions determined from the atmospheric observations. We find impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions, they can neither account for the lingering global CFC-115 emissions determined from the atmospheric observations nor for their recent increases. We also conduct regional inversions for the years 2012–2016 for the northeastern Asian area using observations from the Korean AGAGE site at Gosan and find significant emissions for ΣCFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in northeastern Asia and more specifically on the Chinese mainland.

2018

Modeling the Dynamic Behavior of Radiocesium in Grazing Reindeer

Skuterud, Lavrans; Hevrøy, Tanya Helena; Thørring, Håvard; Ytre-Eide, Martin

Radiocesium contamination in Norwegian reindeer and the factors influencing contamination levels have been studied for more than 50 years, providing significant amounts of data. Monitoring contamination in reindeer is of utmost importance for reindeer husbandry and herders in Norway and will need to be studied for many years because of the persistent contamination levels due to the 1986 Chernobyl fallout. This paper presents a novel dynamic model that takes advantage of the large data sets that have been collected for reindeer monitoring to estimate 137Cs in reindeer meat at any given time. The model has been validated using detailed 137Cs data from one of the herds most affected by the fallout. The model basis includes detailed 137Cs soil data from aerial surveys, GPS-based knowledge of reindeer migration, and local soil-to-vegetation 137Cs transfer information. The validation exercise shows that the model satisfactorily predicts both short- and long-term changes in 137Cs concentrations in reindeer meat and suggests that the model will be a useful tool in estimating seasonal changes and evaluating possible remedial actions in case of a future fallout event.

2022

Mapping potential conflicts between global agriculture and terrestrial conservation

Kanemoto, Keiichiro; Moran, Daniel Dean

Demand for food products, often from international trade, has brought agricultural land use into direct competition with biodiversity. Where these potential conflicts occur and which consumers are responsible is poorly understood. By combining conservation priority (CP) maps with agricultural trade data, we estimate current potential conservation risk hotspots driven by 197 countries across 48 agricultural products. Globally, a third of agricultural production occurs in sites of high CP (CP > 0.75, max = 1.0). While cattle, maize, rice, and soybean pose the greatest threat to very high-CP sites, other low-conservation risk products (e.g., sugar beet, pearl millet, and sunflower) currently are less likely to be grown in sites of agriculture–conservation conflict. Our analysis suggests that a commodity can cause dissimilar conservation threats in different production regions. Accordingly, some of the conservation risks posed by different countries depend on their demand and sourcing patterns of agricultural commodities. Our spatial analyses identify potential hotspots of competition between agriculture and high-conservation value sites (i.e., 0.5° resolution, or ~367 to 3,077km2, grid cells containing both agriculture and high-biodiversity priority habitat), thereby providing additional information that could help prioritize conservation activities and safeguard biodiversity in individual countries and globally. A web-based GIS tool at https://agriculture.spatialfootprint.com/biodiversity/ systematically visualizes the results of our analyses.

2023

FLEXPART v10.1 simulation of source contributions to Arctic black carbon

Zhu, Chunmao; Kanaya, Yugo; Takigawa, Masayuki; Ikeda, Kohei; Tanimoto, Hiroshi; Taketani, Fumikazu; Miyakawa, Takuma; Kobayashi, Hideki; Pisso, Ignacio

The Arctic environment is undergoing rapid changes such as faster warming than the global average and exceptional melting of glaciers in Greenland. Black carbon (BC) particles, which are a short-lived climate pollutant, are one cause of Arctic warming and glacier melting. However, the sources of BC particles are still uncertain. We simulated the potential emission sensitivity of atmospheric BC present over the Arctic (north of 66∘ N) using the FLEXPART (FLEXible PARTicle) Lagrangian transport model (version 10.1). This version includes a new aerosol wet removal scheme, which better represents particle-scavenging processes than older versions did. Arctic BC at the surface (0–500 m) and high altitudes (4750–5250 m) is sensitive to emissions in high latitude (north of 60∘ N) and mid-latitude (30–60∘ N) regions, respectively. Geospatial sources of Arctic BC were quantified, with a focus on emissions from anthropogenic activities (including domestic biofuel burning) and open biomass burning (including agricultural burning in the open field) in 2010. We found that anthropogenic sources contributed 82 % and 83 % of annual Arctic BC at the surface and high altitudes, respectively. Arctic surface BC comes predominantly from anthropogenic emissions in Russia (56 %), with gas flaring from the Yamalo-Nenets Autonomous Okrug and Komi Republic being the main source (31 % of Arctic surface BC). These results highlight the need for regulations to control BC emissions from gas flaring to mitigate the rapid changes in the Arctic environment. In summer, combined open biomass burning in Siberia, Alaska, and Canada contributes 56 %–85 % (75 % on average) and 40 %–72 % (57 %) of Arctic BC at the surface and high altitudes, respectively. A large fraction (40 %) of BC in the Arctic at high altitudes comes from anthropogenic emissions in East Asia, which suggests that the rapidly growing economies of developing countries could have a non-negligible effect on the Arctic. To our knowledge, this is the first year-round evaluation of Arctic BC sources that has been performed using the new wet deposition scheme in FLEXPART. The study provides a scientific basis for actions to mitigate the rapidly changing Arctic environment.

2020

Wetland emission and atmospheric sink changes explain methane growth in 2020

Peng, Shushi; Lin, Xin; Thompson, Rona Louise; Xi, Yi; Liu, Gang; Hauglustaine, Didier; Lan, Xin; Poulter, Benjamin; Ramonet, Michel; Saunois, Marielle; Yin, Yi; Zhang, Zhen; Zheng, Bo; Ciais, Philippe

Atmospheric methane growth reached an exceptionally high rate of 15.1 ± 0.4 parts per billion per year in 2020 despite a probable decrease in anthropogenic methane emissions during COVID-19 lockdowns. Here we quantify changes in methane sources and in its atmospheric sink in 2020 compared with 2019. We find that, globally, total anthropogenic emissions decreased by 1.2 ± 0.1 teragrams of methane per year (Tg CH4 yr−1), fire emissions decreased by 6.5 ± 0.1 Tg CH4 yr−1 and wetland emissions increased by 6.0 ± 2.3 Tg CH4 yr−1. Tropospheric OH concentration decreased by 1.6 ± 0.2 per cent relative to 2019, mainly as a result of lower anthropogenic nitrogen oxide (NOx) emissions and associated lower free tropospheric ozone during pandemic lockdowns. From atmospheric inversions, we also infer that global net emissions increased by 6.9 ± 2.1 Tg CH4 yr−1 in 2020 relative to 2019, and global methane removal from reaction with OH decreased by 7.5 ± 0.8 Tg CH4 yr−1. Therefore, we attribute the methane growth rate anomaly in 2020 relative to 2019 to lower OH sink (53 ± 10 per cent) and higher natural emissions (47 ± 16 per cent), mostly from wetlands. In line with previous findings, our results imply that wetland methane emissions are sensitive to a warmer and wetter climate and could act as a positive feedback mechanism in the future. Our study also suggests that nitrogen oxide emission trends need to be taken into account when implementing the global anthropogenic methane emissions reduction pledge.

2022

Archetypes of Spatial Concentration Variability of Organic Contaminants in the Atmosphere: Implications for Identifying Sources and Mapping the Gaseous Outdoor Inhalation Exposome

Zhan, Faqiang; Li, Yuening; Shunthirasingham, Chubashini; Oh, Jenny; Lei, Ying Duan; Lu, Zhe; Chaaben, Amina Ben; Lee, Kelsey; Gobas, Frank A. P. C.; Hung, Hayley; Breivik, Knut; Wania, Frank

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

Seasonal soil/snow-air exchange of semivolatile organic pollutants at a coastal arctic site (Tromsø, 69°N)

Casal, Paulo; Castro-Jiménez, Javier; Pizarro, Mariana; Katsoyiannis, Athanasios A.; Dachs, Jordi

2018

Comparing national greenhouse gas budgets reported in UNFCCC inventories against atmospheric inversions

Deng, Zhu; Ciais, Philippe; Tzompa-Sosa, Zitely A.; Saunois, Marielle; Qiu, Chunjing; Tan, Chang; Sun, Taochun; Ke, Piyu; Cui, Yanan; Tanaka, Katsumasa; Lin, Xin; Thompson, Rona Louise; Tian, Hanqin; Yao, Yuanzhi; Huang, Yuanyuan; Lauerwald, Ronny; Jain, Atul K.; Xu, Xiaoming; Bastos, Ana; Palmer, Paul I.; Lauvaux, Thomas; d'Aspremont, Alexandre; Giron, Clément; Benoit, Antoine; Poulter, Benjamin; Chang, Jinfeng; Petrescu, Ana Maria Roxana; Davis, Steven J; Liu, Zhu; Grassi, Giacomo; Albergel, Clement; Tubiello, Francesco N.; Perugini, Lucia; Peters, Wouter; Chevallier, Frederic

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

Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo

Hamer, Paul David; Marécal, Virginie; Hossaini, Ryan; Pirre, Michel; Krysztofiak, Gisele; Ziska, Franziska; Engel, Andreas; Sala, Stephan; Keber, Timo; Bönisch, Harald; Atlas, Elliot; Krüger, Kirstin; Chipperfield, Martyn; Catoire, Valery; Samah, Azizan A.; Dorf, Marcel; Moi, Phang Siew; Schlager, Hans; Pfeilsticker, Klaus

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

Lamotte, Claire; Guth, Jonathan; Marécal, Virginie; Cussac, Martin; Hamer, Paul David; Theys, Nicolas; Schneider, Philipp

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

Assessment of Low-Cost Particulate Matter Sensor Systems against Optical and Gravimetric Methods in a Field Co-Location in Norway

Vogt, Matthias; Schneider, Philipp; Castell, Nuria; Hamer, Paul David

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

Six-week inhalation of CdO nanoparticles in mice: The effects on immune response, oxidative stress, antioxidative defense, fibrotic response, and bones

Tulinska, Jana; Masanova, Vlasta; Liskova, Aurelia; Mikusova, Miroslava Lehotska; Rollerova, Eva; Krivosikova, Zora; Stefikova, Kornelia; Uhnakova, Iveta; Ursinyova, Monika; Babickova, Janka; Bábelová, Andrea; Busova, Milena; Tothova, Lubomira; Wsolova, Ladislava; Dusinska, Maria; Sojka, Martin; Horvathova, Mira; Alacova, Radka; Vecera, Zbynek; Mikuska, Pavel; Coufalik, Pavel; Krumal, Kamil; Capka, Lukas; Docekal, Bohumil

2019

Can plastic related chemicals be indicators of plastic ingestion in an Arctic seabird?

Collard, France; Tulatz, Felix; Harju, Mikael; Herzke, Dorte; Bourgeon, Sophie; Gabrielsen, Geir Wing

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

Cassiani, Massimo; Bertagni, Matteo B.; Marro, Massimo; Salizzoni, Pietro

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

Kjølerbakken, Kai Morgan; Miloch, Wojciech Jacek; Røed, Ketil

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

Economic Feasibility of Power/Heat Cogeneration by Biogas–Solid Oxide Fuel Cell (SOFC) Integrated Systems

Athanasiou, Costas; Drosakis, Christos; Booto, Gaylord Kabongo; Elmasides, Costas

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

Cioni, Lara; Nikiforov, Vladimir; Coelho, Ana Carolina Miranda Fernandes; Sandanger, Torkjel M; Herzke, Dorte

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

DNA Damage in Arctic Seabirds: Baseline, Sensitivity to a Genotoxic Stressor, and Association with Organohalogen Contaminants

Haarr, Ane; Hylland, Ketil; Eckbo, Norith; Gabrielsen, Geir W.; Herzke, Dorte; Bustnes, Jan Ove; Blévin, Pierre; Chastel, Olivier; Moe, Børge; Hanssen, Sveinn Are; Sagerup, Kjetil; Borgå, Katrine

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

Schneider, Philipp; Vogt, Matthias; Haugen, Rolf; Hassani, Amirhossein; Castell, Nuria; Dauge, Franck Rene; Bartonova, Alena

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

Aun, Margit; Lakkala, Kaisa; Sanchez, Ricardo; Asmi, Eija; Nollas, Fernando; Meinander, Outi; Sogacheva, Larisa; Bock, Veerle De; Arola, Antti; Leeuw, Gerrit de; Aaltonen, Veijo; Bolsee, David; Cizkova, Klara; Mangold, Alexander; Metelka, Ladislav; Jakobson, Erko; Svendby, Tove Marit; Gillotay, Didier; Opstal, Bert Van

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

Hassani, Amirhossein; Azapagic, Adisa; Shokri, Nima

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

Source term determination with elastic plume bias correction

Tichý, Ondřej; Šmídl, Václav; Evangeliou, Nikolaos

2022

Carbon and Greenhouse Gas Budgets of Europe: Trends, Interannual and Spatial Variability, and Their Drivers

Lauerwald, Ronny; Bastos, Ana; McGrath, Matthew J.; Petrescu, Ana Maria Roxana; Ritter, François; Andrew, Robbie; Berchet, Antoine; Broquet, Grégoire; Brunner, Dominik; Chevallier, Frédéric; Cescatti, Alessandro; Filipek, Sara; Fortems-Cheiney, Audrey; Forzieri, Giovanni; Friedlingstein, Pierre; Fuchs, Richard; Gerbig, Christoph; Houweling, Sanne; Ke, Piyu; Lerink, Bas J. W.; Li, Wanjing; Li, Wei; Li, Xiaojun; Luijkx, Ingrid; Monteil, Guillaume; Munassar, Saqr; Nabuurs, Gert-Jan; Patra, Prabir K.; Peylin, Philippe; Pongratz, Julia; Regnier, Pierre; Saunois, Marielle; Schelhaas, Mart-Jan; Scholze, Marko; Sitch, Stephen; Thompson, Rona Louise; Tian, Hanqin; Tsuruta, Aki; Wilson, Chris; Wigneron, Jean-Pierre; Yao, Yitong; Zaehle, Sönke; Ciais, Philippe

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

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