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Introducing a nested multimedia fate and transport model for organic contaminants (NEM)
Some organic contaminants, including the persistent organic pollutants (POPs), have achieved global distribution through long range atmospheric transport (LRAT). Regulatory efforts, monitoring programs and modelling studies address the LRAT of POPs on national, continental (e.g. Europe) and/or global scales. Whereas national and continental-scale models require estimates of the input of globally dispersed chemicals from outside of the model domain, existing global-scale models either have relatively coarse spatial resolution or are so computationally demanding that it limits their usefulness. Here we introduce the Nested Exposure Model (NEM), which is a multimedia fate and transport model that is global in scale yet can achieve high spatial resolution of a user-defined target region without huge computational demands. Evaluating NEM by comparing model predictions for PCB-153 in air with measurements at nine long-term monitoring sites of the European Monitoring and Evaluation Programme (EMEP) reveals that nested simulations at a resolution of 1° × 1° yield results within a factor of 1.5 of observations at sites in northern Europe. At this resolution, the model attributes more than 90% of the atmospheric burden within any of the grid cells containing an EMEP site to advective atmospheric transport from elsewhere. Deteriorating model performance with decreasing resolution (15° × 15°, 5° × 5° and 1° × 1°), manifested by overestimation of concentrations across most of northern Europe by more than a factor of 3, illustrates the effect of numerical diffusion. Finally, we apply the model to demonstrate how the choice of spatial resolution affect predictions of atmospheric deposition to the Baltic Sea. While we envisage that NEM may be used for a wide range of applications in the future, further evaluation will be required to delineate the boundaries of applicability towards chemicals with divergent fate properties as well as in environmental media other than air.
Royal Society of Chemistry (RSC)
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.
MDPI
2021
Black Carbon Emission Reduction Due to COVID-19 Lockdown in China
American Geophysical Union (AGU)
2021
Integrated water vapor during rain and rain-free conditions above the Swiss Plateau
Water vapor column density, or vertically-integrated water vapor (IWV), is monitored by ground-based microwave radiometers (MWR) and ground-based receivers of the Global Navigation Satellite System (GNSS). For rain periods, the retrieval of IWV from GNSS Zenith Wet Delay (ZWD) neglects the atmospheric propagation delay of the GNSS signal by rain droplets. Similarly, it is difficult for ground-based dual-frequency single-polarisation microwave radiometers to separate the microwave emission of water vapor and cloud droplets from the rather strong microwave emission of rain. For ground-based microwave radiometry at Bern (Switzerland), we take the approach that IWV during rain is derived from linearly interpolated opacities before and after the rain period. The intermittent rain periods often appear as spikes in the time series of integrated liquid water (ILW) and are indicated by ILW ≥ 0.4 mm. In the present study, we assume that IWV measurements from radiosondes are not affected by rain. We intercompare the climatologies of IWV(rain), IWV(no rain), and IWV(all) obtained by radiosonde, ground-based GNSS atmosphere sounding, ground-based MWR, and ECMWF reanalysis (ERA5) at Payerne and Bern in Switzerland. In all seasons, IWV(rain) is 3.75 to 5.94 mm greater than IWV(no rain). The mean IWV differences between GNSS and radiosonde at Payerne are less than 0.26 mm. The datasets at Payerne show a better agreement than the datasets at Bern. However, the MWR at Bern agrees with the radiosonde at Payerne within 0.41 mm for IWV(rain) and 0.02 mm for IWV(no rain). Using the GNSS and rain gauge measurements at Payerne, we find that IWV(rain) increases with increase of the precipitation rate during summer as well as during winter. IWV(rain) above the Swiss Plateau is quite well estimated by GNSS and MWR though the standard retrievals are limited or hampered during rain periods.
MDPI
2021
The influence of probe spacing and probe bias in a double Langmuir probe setup
Multi-needle Langmuir probes are mounted on satellites and sounding rockets for high-frequency characterization of plasma in the ionosphere. Mounted on a spacecraft, the recorded probe current often differs from expected results. In this paper, we perform a numerical study using a particle in cell model to see how the spacing between the individual probes used in a multi-needle setup influences the measured current. We also study how the applied probe bias voltage can contribute to deviations. In our study, we use realistic electron temperatures and electron densities for the relevant part of the ionosphere. However, the results should be generally applicable and valid for other space environments as well as for laboratory Langmuir probe applications. From our study, we can see that when the distance is short, less than two Debye lengths, the current is highly affected, and we can see deviations of more than 60% compared to a single probe setup.
AIP Publishing (American Institute of Physics)
2021
DNA Repair Gene Polymorphisms and Chromosomal Aberrations in Exposed Populations
DNA damage and unrepaired or insufficiently repaired DNA double-strand breaks as well as telomere shortening contribute to the formation of structural chromosomal aberrations (CAs). Non-specific CAs have been used in the monitoring of individuals exposed to potential carcinogenic chemicals and radiation. The frequency of CAs in peripheral blood lymphocytes (PBLs) has been associated with cancer risk and the association has also been found in incident cancer patients. CAs include chromosome-type aberrations (CSAs) and chromatid-type aberrations (CTAs) and their sum CAtot. In the present study, we used data from our published genome-wide association studies (GWASs) and extracted the results for 153 DNA repair genes for 607 persons who had occupational exposure to diverse harmful substances/radiation and/or personal exposure to tobacco smoking. The analyses were conducted using linear and logistic regression models to study the association of DNA repair gene polymorphisms with CAs. Considering an arbitrary cutoff level of 5 × 10–3, 14 loci passed the threshold, and included 7 repair pathways for CTA, 4 for CSA, and 3 for CAtot; 10 SNPs were eQTLs influencing the expression of the target repair gene. For the base excision repair pathway, the implicated genes PARP1 and PARP2 encode poly(ADP-ribosyl) transferases with multiple regulatory functions. PARP1 and PARP2 have an important role in maintaining genome stability through diverse mechanisms. Other candidate genes with known roles for CSAs included GTF2H (general transcription factor IIH subunits 4 and 5), Fanconi anemia pathway genes, and PMS2, a mismatch repair gene. The present results suggest pathways with mechanistic rationale for the formation of CAs and emphasize the need to further develop techniques for measuring individual sensitivity to genotoxic exposure.
Frontiers Media S.A.
2021
How Atmospheric Chemistry and Transport Drive Surface Variability of N2O and CFC-11
American Geophysical Union (AGU)
2021
2021
Taylor & Francis
2021
SAMIRA-SAtellite Based Monitoring Initiative for Regional Air Quality
The satellite based monitoring initiative for regional air quality (SAMIRA) initiative was set up to demonstrate the exploitation of existing satellite data for monitoring regional and urban scale air quality. The project was carried out between May 2016 and December 2019 and focused on aerosol optical depth (AOD), particulate matter (PM), nitrogen dioxide (NO2), and sulfur dioxide (SO2). SAMIRA was built around several research tasks: 1. The spinning enhanced visible and infrared imager (SEVIRI) AOD optimal estimation algorithm was improved and geographically extended from Poland to Romania, the Czech Republic and Southern Norway. A near real-time retrieval was implemented and is currently operational. Correlation coefficients of 0.61 and 0.62 were found between SEVIRI AOD and ground-based sun-photometer for Romania and Poland, respectively. 2. A retrieval for ground-level concentrations of PM2.5 was implemented using the SEVIRI AOD in combination with WRF-Chem output. For representative sites a correlation of 0.56 and 0.49 between satellite-based PM2.5 and in situ PM2.5 was found for Poland and the Czech Republic, respectively. 3. An operational algorithm for data fusion was extended to make use of various satellite-based air quality products (NO2, SO2, AOD, PM2.5 and PM10). For the Czech Republic inclusion of satellite data improved mapping of NO2 in rural areas and on an annual basis in urban background areas. It slightly improved mapping of rural and urban background SO2. The use of satellites based AOD or PM2.5 improved mapping results for PM2.5 and PM10. 4. A geostatistical downscaling algorithm for satellite-based air quality products was developed to bridge the gap towards urban-scale applications. Initial testing using synthetic data was followed by applying the algorithm to OMI NO2 data with a direct comparison against high-resolution TROPOMI NO2 as a reference, thus allowing for a quantitative assessment of the algorithm performance and demonstrating significant accuracy improvements after downscaling. We can conclude that SAMIRA demonstrated the added value of using satellite data for regional- and urban-scale air quality monitoring.
MDPI
2021
Seasonal Variation of Wet Deposition of Black Carbon at Ny-Ålesund, Svalbard
American Geophysical Union (AGU)
2021
Growing Atmospheric Emissions of Sulfuryl Fluoride
American Geophysical Union (AGU)
2021
Observed and Modeled Black Carbon Deposition and Sources in the Western Russian Arctic 1800−2014
Black carbon (BC) particles contribute to climate warming by heating the atmosphere and reducing the albedo of snow/ice surfaces. The available Arctic BC deposition records are restricted to the Atlantic and North American sectors, for which previous studies suggest considerable spatial differences in trends. Here, we present first long-term BC deposition and radiocarbon-based source apportionment data from Russia using four lake sediment records from western Arctic Russia, a region influenced by BC emissions from oil and gas production. The records consistently indicate increasing BC fluxes between 1800 and 2014. The radiocarbon analyses suggest mainly (∼70%) biomass sources for BC with fossil fuel contributions peaking around 1960–1990. Backward calculations with the atmospheric transport model FLEXPART show emission source areas and indicate that modeled BC deposition between 1900 and 1999 is largely driven by emission trends. Comparison of observed and modeled data suggests the need to update anthropogenic BC emission inventories for Russia, as these seem to underestimate Russian BC emissions and since 1980s potentially inaccurately portray their trend. Additionally, the observations may indicate underestimation of wildfire emissions in inventories. Reliable information on BC deposition trends and sources is essential for design of efficient and effective policies to limit climate warming.
2021
Main sources controlling atmospheric burdens of persistent organic pollutants on a national scale
National long-term monitoring programs on persistent organic pollutants (POPs) in background air have traditionally relied on active air sampling techniques. Due to limited spatial coverage of active air samplers, questions remain (i) whether active air sampler monitoring sites are representative for atmospheric burdens within the larger geographical area targeted by the monitoring programs, and thus (ii) if the main sources affecting POPs in background air across a nation are understood. The main objective of this study was to explore the utility of spatial and temporal trends in concert with multiple modelling approaches to understand the main sources affecting polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in background air across a nation. For this purpose, a comprehensive campaign was carried out in summer 2016, measuring POPs in background air across Norway using passive air sampling. Results were compared to a similar campaign in 2006 to assess possible changes over one decade. We furthermore used the Global EMEP Multi-media Modeling System (GLEMOS) and the Flexible Particle dispersion model (FLEXPART) to predict and evaluate the relative importance of primary emissions, secondary emissions, long-range atmospheric transport (LRAT) and national emissions in controlling atmospheric burdens of PCB-153 on a national scale. The concentrations in air of both PCBs and most of the targeted OCPs were generally low, with the exception of hexachlorobenzene (HCB). A limited spatial variability for all POPs in this study, together with predictions by both models, suggest that LRAT dominates atmospheric burdens across Norway. Model predictions by the GLEMOS model, as well as measured isomeric ratios, further suggest that LRAT of some POPs are dictated by secondary emissions. Our results illustrate the utility of combining observations and mechanistic modelling approaches to help identify the main factors affecting atmospheric burdens of POPs across a nation, which, in turn, may be used to inform both national monitoring and control strategies.
Academic Press
2021
Microfibers (MF) are one of the major classes of microplastic found in the marine environment on a global scale. Very little is known about how they move and distribute from point sources such as wastewater effluents into the ocean. We chose Adventfjorden near the settlement of Longyearbyen on the Arctic Svalbard archipelago as a case study to investigate how microfibers emitted with untreated wastewater will distribute in the fjord, both on a spatial and temporal scale. Fiber abundance in the effluent was estimated from wastewater samples taken during two one-week periods in June and September 2017. Large emissions of MFs were detected, similar in scale to a modern WWTP serving 1.3 million people and providing evidence of the importance of untreated wastewater from small settlements as major local sources for MF emissions in the Arctic. Fiber movement and distribution in the fjord mapped using an online-coupled hydrodynamic-drift model (FVCOM-FABM). For parameterizing a wider spectrum of fibers from synthetic to wool, four different density classes of MFs, i.e., buoyant, neutral, sinking, and fast sinking fibers are introduced to the modeling framework. The results clearly show that fiber class has a large impact on the fiber distributions. Light fibers remained in the surface layers and left the fjord quickly with outgoing currents, while heavy fibers mostly sank to the bottom and deposited in the inner parts of the fjord and along the northern shore. A number of accumulation sites were identified within the fjord. The southern shore, in contrast, was much less affected, with low fiber concentrations throughout the modeling period. Fiber distributions were then compared with published pelagic and benthic fauna distributions in different seasons at selected stations around the fjord. The ratios of fibers to organisms showed a very wide range, indicating hot spots of encounter risk for pelagic and benthic biota. This approach, in combination with in-situ ground-truthing, can be instrumental in understanding microplastic pathways and fate in fjord systems and coastal areas and help authorities develop monitoring and mitigation strategies for microfiber and microplastic pollution in their local waters.
Frontiers Media S.A.
2021
2021
2021
2021
Eastward-propagating planetary waves prior to the January 2009 sudden stratospheric warming
American Geophysical Union (AGU)
2021
2021
2021
2021