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2019
Although aerosols in the Arctic have multiple and complex impacts on the regional climate, their removal due to deposition is still not well quantified. We combined meteorological, aerosol, precipitation, and snowpack observations with simulations to derive information about the deposition of sea salt components and black carbon (BC) from November 2011 to April 2012 to the Arctic snowpack at two locations close to Ny-Ålesund, Svalbard. The dominating role of sea salt and the contribution of dust for the composition of atmospheric aerosols were reflected in the seasonal composition of the snowpack. The strong alignment of the concentrations of the major sea salt components in the aerosols, the precipitation, and the snowpack is linked to the importance of wet deposition for transfer from the atmosphere to the snowpack. This agreement was less strong for monthly snow budgets and deposition, indicating important relocation of the impurities inside the snowpack after deposition. Wet deposition was less important for the transfer of nitrate, non-sea-salt sulfate, and BC to the snow during the winter period. The average BC concentration in the snowpack remains small, with a limited impact on snow albedo and melting. Nevertheless, the observations also indicate an important redistribution of BC in the snowpack, leading to layers with enhanced concentrations. The complex behavior of bromide due to modifications during sea salt aerosol formation and remobilization in the atmosphere and in the snow were not resolved because of the lack of bromide measurements in aerosols and precipitation.
2019
2019
2019
We present here emissions estimated from a newly developed emission model for residential wood combustion (RWC) at high spatial and temporal resolution, which we name the MetVed model. The model estimates hourly emissions resolved on a 250 m grid resolution for several compounds, including particulate matter (PM), black carbon (BC) and polycyclic aromatic hydrocarbons (PAHs) in Norway for a 12-year period. The model uses novel input data and calculation methods that combine databases built with an unprecedented high level of detail and near-national coverage. The model establishes wood burning potential at the grid based on the dependencies between variables that influence emissions: i.e. outdoor temperature, number of and type and size of dwellings, type of available heating technologies, distribution of wood-based heating installations and their associated emission factors. RWC activity with a 1 h temporal profile was produced by combining heating degree day and hourly and weekday activity profiles reported by wood consumers in official statistics. This approach results in an improved characterisation of the spatio-temporal distribution of wood use, and subsequently of emissions, required for urban air quality assessments. Whereas most variables are calculated based on bottom-up approaches on a 250 m spatial grid, the MetVed model is set up to use official wood consumption at the county level and then distributes consumption to individual grids proportional to the physical traits of the residences within it. MetVed combines consumption with official emission factors that makes the emissions also upward scalable from the 250 m grid to the national level.
The MetVed spatial distribution obtained was compared at the urban scale to other existing emissions at the same scale. The annual urban emissions, developed according to different spatial proxies, were found to have differences up to an order of magnitude. The MetVed total annual PM2.5 emissions in the urban domains compare well to emissions adjusted based on concentration measurements. In addition, hourly PM2.5 concentrations estimated by an Eulerian dispersion model using MetVed emissions were compared to measurements at air quality stations. Both hourly daily profiles and the seasonality of PM2.5 show a slight overestimation of PM2.5 levels. However, a comparison with black carbon from biomass burning and benzo(a)pyrene measurements indicates higher emissions during winter than that obtained by MetVed. The accuracy of urban emissions from RWC relies on the accuracy of the wood consumption (activity data), emission factors and the spatio-temporal distribution. While there are still knowledge gaps regarding emissions, MetVed represents a vast improvement in the spatial and temporal distribution of RWC.
2019
This paper describes the CityChem extension of the Eulerian urban dispersion model EPISODE. The development of the CityChem extension was driven by the need to apply the model in largely populated urban areas with highly complex pollution sources of particulate matter and various gaseous pollutants. The CityChem extension offers a more advanced treatment of the photochemistry in urban areas and entails specific developments within the sub-grid components for a more accurate representation of dispersion in proximity to urban emission sources. Photochemistry on the Eulerian grid is computed using a numerical chemistry solver. Photochemistry in the sub-grid components is solved with a compact reaction scheme, replacing the photo-stationary-state assumption. The simplified street canyon model (SSCM) is used in the line source sub-grid model to calculate pollutant dispersion in street canyons. The WMPP (WORM Meteorological Pre-Processor) is used in the point source sub-grid model to calculate the wind speed at plume height. The EPISODE–CityChem model integrates the CityChem extension in EPISODE, with the capability of simulating the photochemistry and dispersion of multiple reactive pollutants within urban areas. The main focus of the model is the simulation of the complex atmospheric chemistry involved in the photochemical production of ozone in urban areas. The ability of EPISODE–CityChem to reproduce the temporal variation of major regulated pollutants at air quality monitoring stations in Hamburg, Germany, was compared to that of the standard EPISODE model and the TAPM (The Air Pollution Model) air quality model using identical meteorological fields and emissions. EPISODE–CityChem performs better than EPISODE and TAPM for the prediction of hourly NO2 concentrations at the traffic stations, which is attributable to the street canyon model. Observed levels of annual mean ozone at the five urban background stations in Hamburg are captured by the model within ±15 %. A performance analysis with the FAIRMODE DELTA tool for air quality in Hamburg showed that EPISODE–CityChem fulfils the model performance objectives for NO2 (hourly), O3 (daily max. of the 8 h running mean) and PM10 (daily mean) set forth in the Air Quality Directive, qualifying the model for use in policy applications. Envisaged applications of the EPISODE–CityChem model are urban air quality studies, emission control scenarios in relation to traffic restrictions and the source attribution of sector-specific emissions to observed levels of air pollutants at urban monitoring stations.
2019
2019
Levels and trends of poly- and perfluoroalkyl substances in the Arctic environment – An update
Poly- and perfluoroalkyl substances (PFASs) are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife. Previous reviews by Butt et al. and Letcher et al. have covered studies on levels and trends of PFASs in the Arctic that were available to 2009. The purpose of this review is to focus on more recent work, generally published between 2009 and 2018, with emphasis on PFASs of emerging concern such as perfluoroalkyl carboxylates (PFCAs) and short-chain perfluoroalkyl sulfonates (PFSAs) and their precursors. Atmospheric measurements over the period 2006–2014 have shown that fluorotelomer alcohols (FTOHs) as well as perfluorobutanoic acid (PFBA) and perfluoroctanoic acid (PFOA) are the most prominent PFASs in the arctic atmosphere, all with increasing concentrations at Alert although PFOA concentrations declined at the Zeppelin Station (Svalbard). Results from ice cores show generally increasing deposition of PFCAs on the Devon Ice cap in the Canadian arctic while declining fluxes were found in a glacier on Svalbard. An extensive dataset exists for long-term trends of long-chain PFCAs that have been reported in Arctic biota with some datasets including archived samples from the 1970s and 1980s. Trends in PFCAs over time vary among the same species across the North American Arctic, East and West Greenland, and Svalbard. Most long term time series show a decline from higher concentrations in the early 2000s. However there have been recent (post 2010) increasing trends of PFCAs in ringed seals in the Canadian Arctic, East Greenland polar bears and in arctic foxes in Svalbard. Annual biological sampling is helping to determine these relatively short term changes. Rising levels of some PFCAs have been explained by continued emissions of long-chain PFCAs and/or their precursors and inflows to the Arctic Ocean, especially from the North Atlantic. While the effectiveness of biological sampling for temporal trends in long-chain PFCAs and PFSAs has been demonstrated, this does not apply to the C4–C8–PFCAs, perfluorobutane sulfonamide (FBSA), or perfluorobutane sulfonate (PFBS) which are generally present at low concentrations in biota. In addition to air sampling, sampling abiotic media such as glacial cores, and annual sampling of lake waters and seawater would appear to be the best approaches for investigating trends in the less bioaccumulative PFASs.
2019
Socioeconomic position, lifestyle habits and biomarkers of epigenetic aging: A multi-cohort analysis
Differences in health status by socioeconomic position (SEP) tend to be more evident at older ages, suggesting the involvement of a biological mechanism responsive to the accumulation of deleterious exposures across the lifespan. DNA methylation (DNAm) has been proposed as a biomarker of biological aging that conserves memory of endogenous and exogenous stress during life.
We examined the association of education level, as an indicator of SEP, and lifestyle-related variables with four biomarkers of age-dependent DNAm dysregulation: the total number of stochastic epigenetic mutations (SEMs) and three epigenetic clocks (Horvath, Hannum and Levine), in 18 cohorts spanning 12 countries.
The four biological aging biomarkers were associated with education and different sets of risk factors independently, and the magnitude of the effects differed depending on the biomarker and the predictor. On average, the effect of low education on epigenetic aging was comparable with those of other lifestyle-related risk factors (obesity, alcohol intake), with the exception of smoking, which had a significantly stronger effect.
Our study shows that low education is an independent predictor of accelerated biological (epigenetic) aging and that epigenetic clocks appear to be good candidates for disentangling the biological pathways underlying social inequalities in healthy aging and longevity.
2019
2019
The Mineral Aerosol Profiling from Infrared Radiances (MAPIR) algorithm retrieves vertical dust concentration profiles from cloud-free Infrared Atmospheric Sounding Interferometer (IASI) thermal infrared (TIR) radiances using Rodgers' optimal estimation method (OEM). We describe the new version 4.1 and evaluation results. Main differences with respect to previous versions are the Levenberg–Marquardt modification of the OEM, the use of the logarithm of the concentration in the retrieval and the use of Radiative Transfer for TOVS (RTTOV) for in-line radiative transfer calculations. The dust aerosol concentrations are retrieved in seven 1 km thick layers centered at 0.5 to 6.5 km. A global data set of the daily dust distribution was generated with MAPIR v4.1 covering September 2007 to June 2018, with further extensions planned every 6 months. The post-retrieval quality filters reject about 16 % of the retrievals, a huge improvement with respect to the previous versions in which up to 40 % of the retrievals were of bad quality. The median difference between the observed and fitted spectra of the good-quality retrievals is 0.32 K, with lower values over oceans. The information content of the retrieved profiles shows a dependence on the total aerosol load due to the assumption of a lognormal state vector. The median degrees of freedom in dusty scenes (min 10 µm AOD of 0.5) is 1.4. An evaluation of the aerosol optical depth (AOD) obtained from the integrated MAPIR v4.1 profiles was performed against 72 AErosol RObotic NETwork (AERONET) stations. The MAPIR AOD correlates well with the ground-based data, with a mean correlation coefficient of 0.66 and values as high as 0.88. Overall, there is a mean AOD (550 nm) positive bias of only 0.04 with respect to AERONET, which is an extremely good result. The previous versions of MAPIR were known to largely overestimate AOD (about 0.28 for v3). A second evaluation exercise was performed comparing the mean aerosol layer altitude from MAPIR with the mean dust altitude from Cloud–Aerosol LIdar with Orthogonal Polarization (CALIOP). A small underestimation was found, with a mean difference of about 350 m (standard deviation of about 1 km) with respect to the CALIOP cumulative extinction altitude, which is again considered very good as the vertical resolution of MAPIR is 1 km. In the comparisons against AERONET and CALIOP, a dependence of MAPIR on the quality of the temperature profiles used in the retrieval is observed. Finally, a qualitative comparison of dust aerosol concentration profiles was done against lidar measurements from two ground-based stations (M'Bour and Al Dhaid) and from the Cloud–Aerosol Transport System (CATS) instrument on board the International Space Station (ISS). MAPIR v4.1 showed the ability to detect dust plumes at the same time and with a similar extent as the lidar instruments. This new MAPIR version shows a great improvement of the accuracy of the aerosol profile retrievals with respect to previous versions, especially so for the integrated AOD. It now offers a unique 3-D dust data set, which can be used to gain more insight into the transport and emission processes of mineral dust aerosols.
2019
2019
2019
Information on the origin of pollution constitutes an essential step of air quality management as it helps identifying measures to control air pollution. In this work, we review the most widely used source-apportionment methods for air quality management. Using theoretical and real-case datasets we study the differences among these methods and explain why they result in very different conclusions to support air quality planning. These differences are a consequence of the intrinsic assumptions that underpin the different methodologies and determine/limit their range of applicability. We show that ignoring their underlying assumptions is a risk for efficient/successful air quality management as these methods are sometimes used beyond their scope and range of applicability. The simplest approach based on increments (incremental approach) is often not suitable to support air quality planning. Contributions obtained through mass-transfer methods (receptor models or tagging approaches built in air quality models) are appropriate to support planning but only for specific pollutants. Impacts obtained via “brute-force” methods are the best suited but it is important to assess carefully their application range to make sure they reproduce correctly the prevailing chemical regimes.
Elsevier
2019
BACKGROUND: In order to use in situ measurements to constrain urban anthropogenic emissions of carbon dioxide (CO2), we use a Lagrangian methodology based on diffusive backward trajectory tracer reconstructions and Bayesian inversion. The observations of atmospheric CO2 were collected within the Tokyo Bay Area during the Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) flights, from the Tsukuba tall tower of the Meteorological Research Institute (MRI) of the Japan Meteorological Agency and at two surface sites (Dodaira and Kisai) from the World Data Center for Greenhouse Gases (WDCGG).
RESULTS: We produce gridded estimates of the CO2 emissions and calculate the averages for different areas within the Kanto plain where Tokyo is located. Using these inversions as reference we investigate the impact of perturbing different elements in the inversion system. We modified the observations amount and location (surface only sparse vs. including aircraft CO2 observations), the background representation, the wind data used to drive the transport model, the prior emissions magnitude and time resolution and error parameters of the inverse model.
CONCLUSIONS: Optimized fluxes were consistent with other estimates for the unperturbed simulations. Inclusion of CONTRAIL measurements resulted in significant differences in the magnitude of the retrieved fluxes, 13% on average for the whole domain and of up to 21% for the spatiotemporal cells with the highest fluxes. Changes in the background yielded differences in the retrieved fluxes of up to 50% and more. Simulated biases in the modelled transport cause differences in the retrieved fluxes of up to 30% similar to those obtained using different meteorological winds to advect the Lagrangian trajectories. Perturbations to the prior inventory can impact the fluxes by ~ 10% or more depending on the assumptions on the error covariances. All of these factors can cause significant differences in the estimated flux, and highlight the challenges in estimating regional CO2 fluxes from atmospheric observations.
BioMed Central (BMC)
2019
Peroxisome proliferator-activated receptor alfa (PPARA/NR1C1) is a ligand activated nuclear receptor that is a key regulator of lipid metabolism in tissues with high fatty acid catabolism such as the liver. Here, we cloned PPARA from polar bear liver tissue and studied in vitro transactivation of polar bear and human PPARA by environmental contaminants using a luciferase reporter assay. Six hinge and ligand-binding domain amino acids have been substituted in polar bear PPARA compared to human PPARA. Perfluorocarboxylic acids (PFCA) and perfluorosulfonic acids induced the transcriptional activity of both human and polar bear PPARA. The most abundant PFCA in polar bear tissue, perfluorononanoate, increased polar bear PPARA-mediated luciferase activity to a level comparable to that of the potent PPARA agonist WY-14643 (~8-fold, 25 μM). Several brominated flame retardants were weak agonists of human and polar bear PPARA. While single exposures to polychlorinated biphenyls did not, or only slightly, increase the transcriptional activity of PPARA, a technical mixture of PCBs (Aroclor 1254) strongly induced the transcriptional activity of human (~8-fold) and polar bear PPARA (~22-fold). Polar bear PPARA was both quantitatively and qualitatively more susceptible than human PPARA to transactivation by less lipophilic compounds.
Nature Portfolio
2019
American Geophysical Union (AGU)
2019
Global Historical Stocks and Emissions of PBDEs
The first spatially and temporally resolved inventory of BDE28, 47, 99, 153, 183, and 209 in the anthroposphere and environment is presented here. The stock and emissions of PBDE congeners were estimated using a dynamic substance flow analysis model, CiP-CAFE. To evaluate our results, the emission estimates were used as input to the BETR-Global model. Estimated concentrations were compared with observed concentrations in air from background areas. The global (a) in-use and (b) waste stocks of ∑5BDE(28, 47, 99, 153, 183) and BDE209 are estimated to be (a) ∼25 and 400 kt and (b) 13 and 100 kt, respectively, in 2018. A total of 6 (0.3–13) and 10.5 (9–12) kt of ∑5BDE and BDE209, respectively, has been emitted to the atmosphere by 2018. More than 70% of PBDE emissions during production and use occurred in the industrialized regions, while more than 70% of the emissions during waste disposal occurred in the less industrialized regions. A total of 70 kt of ∑5BDE and BDE209 was recycled within products since 1970. As recycling rates are expected to increase under the circular economy, an additional 45 kt of PBDEs (mainly BDE209) may reappear in new products.
2019
Bird feathers as a biomonitor for environmental pollutants: Prospects and pitfalls
Due to increasing amounts of hazardous chemicals released into the environment, there is a high demand for developing easy and non-destructive biomonitoring tools. In a recent paper published in Trends in Analytical Chemistry, Rutkowska et al. (2018) concluded that feathers are a good matrix for biomonitoring of environmental pollutants in birds. In this commentary, we discuss the general conclusion of this paper. We provide several examples for which this statement is not correct, and we emphasize that only for legacy persistent organic pollutants (POPs) and mercury there is currently enough scientific evidence to use feathers as a reliable biomonitor, given that appropriate sampling designs and QA/QC protocols are taken into account. Furthermore, we discuss different pretreatment (e.g. feather washing) and analytical protocols along with specific QA/QC to be considered. In summary, this commentary provides an overview of the prospects and pitfalls when using feathers as a biomonitor for environmental pollutants.
2019
2019
Supporting the improvement of air quality management practices: The “FAIRMODE pilot” activity
This paper presents the first outcomes of the “FAIRMODE pilot” activity, aiming at improving the way in which air quality models are used in the frame of the European “Air Quality Directive”. Member States may use modelling, combined with measurements, to “assess” current levels of air quality and estimate future air quality under different scenarios. In case of current and potential exceedances of the Directive limit values, it is also requested that they “plan” and implement emission reductions measures to avoid future exceedances. In both “assessment” and “planning”, air quality models can and should be used; but to do so, the used modelling chain has to be fit-for-purpose and properly checked and verified. FAIRMODE has developed in the recent years a suite of methodologies and tools to check if emission inventories, model performance, source apportionment techniques and planning activities are fit-for-purpose. Within the “FAIRMODE pilot”, these tools are used and tested by regional/local authorities, with the two-fold objective of improving management practices at regional/local scale, and providing valuable feedback to the FAIRMODE community. Results and lessons learnt from this activity are presented in this paper, as a showcase that can potentially benefit other authorities in charge of air quality assessment and planning.
Elsevier
2019
Monitoring Soil Moisture Drought over Northern High Latitudes from Space
Mapping drought from space using, e.g., surface soil moisture (SSM), has become viable in the last decade. However, state of the art SSM retrieval products suffer from very poor coverage over northern latitudes. In this study, we propose an innovative drought indicator with a wider spatial and temporal coverage than that obtained from satellite SSM retrievals. We evaluate passive microwave brightness temperature observations from the Soil Moisture and Ocean Salinity (SMOS) satellite as a surrogate drought metric, and introduce a Standardized Brightness Temperature Index (STBI). We compute the STBI by fitting a Gaussian distribution using monthly brightness temperature data from SMOS; the normal assumption is tested using the Shapior-Wilk test. Our results indicate that the assumption of normally distributed brightness temperature data is valid at the 0.05 significance level. The STBI is validated against drought indices from a land surface data assimilation system (LDAS-Monde), two satellite derived SSM indices, one from SMOS and one from the ESA CCI soil moisture project and a standardized precipitation index based on in situ data from the European Climate Assessment & Dataset (ECA&D) project. When comparing the temporal dynamics of the STBI to the LDAS-Monde drought index we find that it has equal correlation skill to that of the ESA CCI soil moisture product ( 0.71 ). However, in addition the STBI provides improved spatial coverage because no masking has been applied over regions with dense boreal forest. Finally, we evaluate the STBI in a case study of the 2018 Nordic drought. The STBI is found to provide improved spatial and temporal coverage when compared to the drought index created from satellite derived SSM over the Nordic region. Our results indicate that when compared to drought indices from precipitation data and a land data assimilation system, the STBI is qualitatively able to capture the 2018 drought onset, severity and spatial extent. We did see that the STBI was unable to detect the 2018 drought recovery for some areas in the Nordic countries. This false drought detection is likely linked to the recovery of vegetation after the drought, which causes an increase in the passive microwave brightness temperature, hence the STBI shows a dry anomaly instead of normal conditions, as seen for the other drought indices. We argue that the STBI could provide additional information for drought monitoring in regions where the SSM retrieval problem is not well defined. However, it then needs to be accompanied by a vegetation index to account for the recovery of the vegetation which could cause false drought detection.
MDPI
2019
Using meteor wind data from the Super Dual Auroral Radar Network (SuperDARN) in the Northern Hemisphere, we (1) demonstrate that the migrating (Sun‐synchronous) tides can be separated from the nonmigrating components in the mesosphere and lower thermosphere (MLT) region and (2) use this to determine the response of the different components of the semidiurnal tide (SDT) to sudden stratospheric warming (SSW) conditions. The radars span a limited range of latitudes around 60°N and are located over nearly 180° of longitude. The migrating tide is extracted from the nonmigrating components observed in the meridional wind recorded from meteor ablation drift velocities around 95‐km altitude, and a 20‐year climatology of the different components is presented. The well‐documented late summer and wintertime maxima in the semidiurnal winds are shown to be due primarily to the migrating SDT, whereas during late autumn and spring the nonmigrating components are at least as strong as the migrating SDT. The robust behavior of the SDT components during SSWs is then examined by compositing 13 SSW events associated with an elevated stratopause recorded between 1995 and 2013. The migrating SDT is seen to reduce in amplitude immediately after SSW onset and then return anomalously strongly around 10–17 days after the SSW onset. We conclude that changes in the underlying wind direction play a role in modulating the tidal amplitude during the evolution of SSWs and that the enhancement in the midlatitude migrating SDT (previously reported in modeling studies) is observed in the MLT at least up to 60°N.
American Geophysical Union (AGU)
2019
Recent Trends in Stratospheric Chlorine From Very Short-Lived Substances
Very short‐lived substances (VSLS), including dichloromethane (CH2Cl2), chloroform (CHCl3), perchloroethylene (C2Cl4), and 1,2‐dichloroethane (C2H4Cl2), are a stratospheric chlorine source and therefore contribute to ozone depletion. We quantify stratospheric chlorine trends from these VSLS (VSLCltot) using a chemical transport model and atmospheric measurements, including novel high‐altitude aircraft data from the NASA VIRGAS (2015) and POSIDON (2016) missions. We estimate VSLCltot increased from 69 (±14) parts per trillion (ppt) Cl in 2000 to 111 (±22) ppt Cl in 2017, with >80% delivered to the stratosphere through source gas injection, and the remainder from product gases. The modeled evolution of chlorine source gas injection agrees well with historical aircraft data, which corroborate reported surface CH2Cl2 increases since the mid‐2000s. The relative contribution of VSLS to total stratospheric chlorine increased from ~2% in 2000 to ~3.4% in 2017, reflecting both VSLS growth and decreases in long‐lived halocarbons. We derive a mean VSLCltot growth rate of 3.8 (±0.3) ppt Cl/year between 2004 and 2017, though year‐to‐year growth rates are variable and were small or negative in the period 2015–2017. Whether this is a transient effect, or longer‐term stabilization, requires monitoring. In the upper stratosphere, the modeled rate of HCl decline (2004–2017) is −5.2% per decade with VSLS included, in good agreement to ACE satellite data (−4.8% per decade), and 15% slower than a model simulation without VSLS. Thus, VSLS have offset a portion of stratospheric chlorine reductions since the mid‐2000s.
American Geophysical Union (AGU)
2019