scholarly journals Intercontinental transport of nitrogen oxide pollution plumes

2003 ◽  
Vol 3 (2) ◽  
pp. 387-393 ◽  
Author(s):  
M. Wenig ◽  
N. Spichtinger ◽  
A. Stohl ◽  
G. Held ◽  
S. Beirle ◽  
...  

Abstract. We describe the first satellite observation of intercontinental transport of nitrogen oxides emitted by power plants, verified by simulations with a particle tracer model. The analysis of such episodes shows that anthropogenic NOx plumes may influence the atmospheric chemistry thousands of kilometers away from its origin, as well as the ocean they traverse due to nitrogen fertilization. This kind of monitoring became possible by applying an improved algorithm to extract the tropospheric fraction of NO2 from the spectral data coming from the GOME instrument. As an example we show the observation of NO2 in the time period 4--14 May, 1998, from the South African Plateau to Australia which was possible due to favourable weather conditions during that time period which availed the satellite measurement. This episode was also simulated with the Lagrangian particle dispersion model FLEXPART which uses NOx emissions taken from an inventory for industrial emissions in South Africa and is driven with analyses from the European Centre for Medium-Range Weather Forecasts. Additionally lightning emissions were taken into account by utilizing Lightning Imaging Sensor data. Lightning was found to contribute probably not more than 25% of the resulting concentrations. Both, the measured and simulated emission plume show matching patterns while traversing the Indian Ocean to Australia and show great resemblance to the aerosol and CO2 transport observed by Piketh et al. (2000).

2002 ◽  
Vol 2 (6) ◽  
pp. 2151-2165 ◽  
Author(s):  
M. Wenig ◽  
N. Spichtinger ◽  
A. Stohl ◽  
G. Held ◽  
S. Beirle ◽  
...  

Abstract. We describe the first satellite observation of intercontinental transport of nitrogen oxides emitted by power plants, verified by simulations with a particle tracer model. The analysis of such episodes shows that anthropogenic NOx plumes may influence the atmospheric chemistry thousands of kilometers away from its origin, as well as the ocean they traverse due to nitrogen fertilization. This kind of monitoring became possible by applying an improved algorithm to extract the tropospheric fraction of NO2 from the spectral data coming from the GOME instrument. As an example we show the observation of NO2 in the time period 4--14 May, 1998, from the South African Plateau to Australia which was possible due to favourable weather conditions during that time period which availed the satellite measurement. This episode was also simulated with the Lagrangian particle dispersion model FLEXPART which uses NOx emissions taken from an inventory for industrial emissions in South Africa and is driven with analyses from the European Centre for Medium-Range Weather Forecasts. Additionally lightning emissions were added by utilizing Lightning Imaging Sensor data. Lightning NOx  was found to amount to around 10% of the resulting concentrations. Both, the measured and simulated emission plume show matching patterns while traversing the Indian Ocean to Australia and show great resemblance to the aerosol and CO2 transport observed by Piketh et al. (2000)


2000 ◽  
Vol 123 (2) ◽  
pp. 303-310 ◽  
Author(s):  
J. Anagnostopoulos ◽  
G. Bergeles ◽  
B. Epple ◽  
P. Stegelitz

A numerical algorithm is developed for a detailed 3D simulation of the two-phase flow field in fluid-energy mills used for pulverization and drying of fossil fuels in large power plants. The gas phase equations are solved using finite differences and the control volume method, whereas a Lagrangian formulation with a stochastic particle dispersion model is adopted for the particulate phase. Fluid-particle interaction is taken into account to calculate the mass, momentum, and heat transfer between phases. Advanced numerical techniques for partially-blocked cells and local grid refinement have been utilized to achieve an accurate representation of the domain geometry and to enhance the accuracy of the results. Particle collisions, fragmentation mechanism, and moisture evaporation are simulated by corresponding models, whereas the special treatment employed for the rotating fan region provides the capability to solve the two-phase flow simultaneously in the entire rotating and nonrotating mill domain. The flow and the operation characteristics of a recently developed lignite mill are measured, and the numerical algorithm is used to predict the mill performance under various inlet profiles of the fuel mass flow rate. The predicted results are reasonable, and in agreement with the available measurements and observations, thus offering a deeper insight into the complex dynamic and thermal behavior of the two-phase flow in the mill.


2015 ◽  
Vol 15 (16) ◽  
pp. 9413-9433 ◽  
Author(s):  
S. Eckhardt ◽  
B. Quennehen ◽  
D. J. L. Olivié ◽  
T. K. Berntsen ◽  
R. Cherian ◽  
...  

Abstract. The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of 2 years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC or rBC and sulfate concentrations quite well, compared to previous comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January–March underestimated by 59 and 37 % for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44 % for July–September), but with overestimates as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is 3 times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modeling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution.


2009 ◽  
Vol 9 (10) ◽  
pp. 3371-3383 ◽  
Author(s):  
J. Cui ◽  
M. Sprenger ◽  
J. Staehelin ◽  
A. Siegrist ◽  
M. Kunz ◽  
...  

Abstract. The particle dispersion model FLEXPART and the trajectory model LAGRANTO are Lagrangian models which are widely used to study synoptic-scale atmospheric air flows such as stratospheric intrusions (SI) and intercontinental transport (ICT). In this study, we focus on SI and ICT events particularly from the North American planetary boundary layer for the Jungfraujoch (JFJ) measurement site, Switzerland, in 2005. Two representative cases of SI and ICT are identified based on measurements recorded at Jungfraujoch and are compared with FLEXPART and LAGRANTO simulations, respectively. Both models well capture the events, showing good temporal agreement between models and measurements. In addition, we investigate the performance of FLEXPART and LAGRANTO on representing SI and ICT events over the entire year 2005 in a statistical way. We found that the air at JFJ is influenced by SI during 19% (FLEXPART) and 18% (LAGRANTO), and by ICT from the North American planetary boundary layer during 13% (FLEXPART) and 12% (LAGRANTO) of the entire year. Through intercomparsion with measurements, our findings suggest that both FLEXPART and LAGRANTO are well capable of representing SI and ICT events if they last for more than 12 h, whereas both have problems on representing short events. For comparison with in-situ observations we used O3 and relative humidity for SI events. As parameters to trace ICT events we used a combination of NOy/CO and CO, however these parameters are not specific enough to distinguish aged air masses by their source regions. Moreover, a sensitivity study indicates that the agreement between models and measurements depends significantly on the threshold values applied to the individual control parameters. Generally, the less strict the thresholds are, the better the agreement between models and measurements. Although the dependence of the agreement on the threshold values is appreciable, it nevertheless confirms the conclusion that both FLEXPART and LAGRANTO are well able to capture SI and ICT events with duration longer than 12 h.


2009 ◽  
Vol 9 (6) ◽  
pp. 26095-26142 ◽  
Author(s):  
J. E. Jonson ◽  
A. Stohl ◽  
A. M. Fiore ◽  
P. Hess ◽  
S. Szopa ◽  
...  

Abstract. A multi-model study of the long-range transport of ozone and its precursors from major anthropogenic source regions was coordinated by the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) under the Convention on Long-range Transboundary Air Pollution (LRTAP). Vertical profiles of ozone at 12-h intervals in year 2001 are available from twelve of the models contributing to this study and are compared here with observed profiles from ozonesondes. The contributions from each major source region are analysed for selected sondes, and this analysis is supplemented by retroplume calculations using the FLEXPART Lagrangian particle dispersion model to provide insight into the origin of ozone transport events and the cause of differences between the models and observations. In the boundary layer ozone levels are in general strongly affected by regional sources and sinks. With a considerably longer lifetime in the free troposphere, ozone here is to a much larger extent affected by processes on a larger scale such as intercontinental transport and exchange with the stratosphere. Such individual events are difficult to trace over several days or weeks of transport. As a result statistical relationships between models and ozone sonde measurements are far less satisfactory than for surface measurements at all seasons. The lowest bias between model calculated ozone profiles and the ozone sonde measurements is seen in the winter and autumn months. Following the increase in photochemical activity in the spring and summer months the spread in model results increases and the agreement between ozone sonde measurements and the individual models deteriorates further. At selected sites calculated contributions to ozone levels in the free troposphere from intercontinental transport are presented. Intercontinental transport is identified based on differences in model calculations with unperturbed emissions and emissions reduced by 20% by region. With emissions perturbed by 20% per region calculated intercontinental contributions to ozone in the free troposphere range from less than 1 ppb to 3 ppb, with small contributions in winter. The results are corroborated by the retroplume calculations. At several locations the seasonal contributions to ozone in the free troposphere from intercontinental transport differ from what has been shown earlier at the surface using the same dataset. The large spread in model results points to a need of further evaluation of the chemical and physical processes in order to improve the credibility of global model results.


2015 ◽  
Vol 15 (7) ◽  
pp. 10425-10477 ◽  
Author(s):  
S. Eckhardt ◽  
B. Quennehen ◽  
D. J. L. Olivié ◽  
T. K. Berntsen ◽  
R. Cherian ◽  
...  

Abstract. The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of two years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry-transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry-climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC/rBC and sulfate concentrations quite well, compared to past comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January-March underestimated by 59 and 37% for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44% for July–September), but with over- as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is three times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modelling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution.


2011 ◽  
Vol 4 (2) ◽  
pp. 317-324 ◽  
Author(s):  
Y. Koyama ◽  
S. Maksyutov ◽  
H. Mukai ◽  
K. Thoning ◽  
P. Tans

Abstract. This study assesses the advantages of using a coupled atmospheric-tracer transport model, comprising a global Eulerian model and a global Lagrangian particle dispersion model, to improve the reproducibility of tracer-gas variations affected by the near-field surface emissions and transport around observation sites. The ability to resolve variability in atmospheric composition on an hourly time-scale and a spatial scale of several kilometers would be beneficial for analyzing data from continuous ground-based monitoring and from upcoming space-based observations. The coupled model yields an increase in the horizontal resolution of transport and fluxes, and has been tested in regional-scale studies of atmospheric chemistry. By applying the Lagrangian component to the global domain, we extend this approach to the global scale, thereby enabling computationally efficient global inverse modeling and data assimilation. To validate the coupled model, we compare model-simulated CO2 concentrations with continuous observations at three sites: two operated by the National Oceanic and Atmospheric Administration, USA, and one operated by the National Institute for Environmental Studies, Japan. As the goal of this study is limited to introducing the new modeling approach, we selected a transport simulation at these three sites to demonstrate how the model may perform at various geographical areas. The coupled model provides improved agreement between modeled and observed CO2 concentrations in comparison to the Eulerian model. In an area where variability in CO2 concentration is dominated by a fossil fuel signal, the correlation coefficient between modeled and observed concentrations increases by between 0.05 to 0.1 from the original values of 0.5–0.6 achieved with the Eulerian model.


2010 ◽  
Vol 10 (12) ◽  
pp. 5759-5783 ◽  
Author(s):  
J. E. Jonson ◽  
A. Stohl ◽  
A. M. Fiore ◽  
P. Hess ◽  
S. Szopa ◽  
...  

Abstract. A multi-model study of the long-range transport of ozone and its precursors from major anthropogenic source regions was coordinated by the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) under the Convention on Long-range Transboundary Air Pollution (LRTAP). Vertical profiles of ozone at 12-h intervals from 2001 are available from twelve of the models contributing to this study and are compared here with observed profiles from ozonesondes. The contributions from each major source region are analysed for selected sondes, and this analysis is supplemented by retroplume calculations using the FLEXPART Lagrangian particle dispersion model to provide insight into the origin of ozone transport events and the cause of differences between the models and observations. In the boundary layer ozone levels are in general strongly affected by regional sources and sinks. With a considerably longer lifetime in the free troposphere, ozone here is to a much larger extent affected by processes on a larger scale such as intercontinental transport and exchange with the stratosphere. Such individual events are difficult to trace over several days or weeks of transport. This may explain why statistical relationships between models and ozonesonde measurements are far less satisfactory than shown in previous studies for surface measurements at all seasons. The lowest bias between model-calculated ozone profiles and the ozonesonde measurements is seen in the winter and autumn months. Following the increase in photochemical activity in the spring and summer months, the spread in model results increases, and the agreement between ozonesonde measurements and the individual models deteriorates further. At selected sites calculated contributions to ozone levels in the free troposphere from intercontinental transport are shown. Intercontinental transport is identified based on differences in model calculations with unperturbed emissions and emissions reduced by 20% by region. Intercontinental transport of ozone is finally determined based on differences in model ensemble calculations. With emissions perturbed by 20% per region, calculated intercontinental contributions to ozone in the free troposphere range from less than 1 ppb to 3 ppb, with small contributions in winter. The results are corroborated by the retroplume calculations. At several locations the seasonal contributions to ozone in the free troposphere from intercontinental transport differ from what was shown earlier at the surface using the same dataset. The large spread in model results points to a need of further evaluation of the chemical and physical processes in order to improve the credibility of global model results.


2021 ◽  
Author(s):  
Theresa Klausner ◽  
Heidi Huntrieser ◽  
Heinfried Aufmhoff ◽  
Robert Baumann ◽  
Alina Fiehn ◽  
...  

<p>Sulfur dioxide (SO<sub>2</sub>) is known as a major air pollutant harmful to human health. Furthermore, it is a precursor gas of sulfate aerosol, which exerts a direct negative radiative forcing and thus leads to climate cooling. Anthropogenic SO<sub>2</sub> sources are primarily associated with the combustion of sulfur-rich fossil fuels. While the operation of flue gas desulfurization devices has led to large SO<sub>2</sub> reductions in western Europe, a hotspot of anthropogenic SO<sub>2</sub> sources remains in the Balkan region as recently observed from space by the TROPOMI instrument on the Sentinel-5P satellite. Large coal-fired power plants with no or only incomplete SO<sub>2</sub> removal cause these high emissions.</p><p>Targeting these strong emitters, the DLR Falcon 20 aircraft was equipped with an isotopically on-line calibrated Chemical Ionization Ion Trap Mass Spectrometer (CI-ITMS) to obtain detailed in situ SO<sub>2</sub> observations during the METHANE-To-Go-Europe aircraft campaign in autumn 2020. These SO<sub>2</sub> measurements were complemented by in situ observations of greenhouse gases (CO<sub>2</sub>, CH<sub>4</sub>), aerosol number concentrations, and other short-lived pollutants (CO, NO, NO<sub>y</sub>). Two flights, on November 2<sup>nd</sup> and 7<sup>th</sup> 2020, focused on characterizing the pollution plumes downwind of two coal-fired power plants located in Bosnia-Herzegovina (Tuzla) and Serbia (Nikola Tesla), respectively. These power plants belong to the ten strongest SO<sub>2</sub> emitters in Europe, and according to the World Health Organization, both countries are among the most polluted ones in Europe.</p><p>We present a detailed analysis of the two DLR Falcon flights with strongly enhanced SO<sub>2</sub> mixing ratios (exceeding 50 ppb), which were observed at low flight altitude (<1 km). Respective flight patterns were designed to allow for the evaluation of the TROPOMI vertical SO<sub>2</sub> column densities, and both flights were performed during cloud-free conditions. The airborne measurements and satellite data will also be complemented by hourly ground-based SO<sub>2</sub> measurements near both power plants. In addition, measurements are combined with state-of-the art model simulations from (i) the regional atmospheric chemistry climate model MECO(n); (ii) the atmospheric transport and dispersion model HYSPLIT; and (iii) the chemistry coupled Weather Research and Forecasting model WRF-Chem to improve the emission quantification of these power plants.</p>


2009 ◽  
Vol 9 (1) ◽  
pp. 1447-1487
Author(s):  
J. Cui ◽  
M. Sprenger ◽  
J. Staehelin ◽  
A. Siegrist ◽  
M. Kunz ◽  
...  

Abstract. The particle dispersion model FLEXPART and the trajectory model LAGRANTO are Lagrangian models which are widely used to study synoptic-scale atmospheric air flows such as stratospheric intrusions (SI) and intercontinental transport (ICT). In this study, we focus on SI and ICT events particularly from the North American planetary boundary layer for the Jungfraujoch (JFJ) measurement site, Switzerland, in 2005. Two representative cases of SI and ICT are identified based on measurements recorded at Jungfraujoch and are compared with FLEXPART and LAGRANTO simulations, respectively. Both models well capture the events, showing good temporal agreement between models and measurements. In addition, we investigate the performance of FLEXPART and LAGRANTO on representing SI and ICT events over the entire year 2005 in a statistical way. We found that the air at JFJ is influenced by SI during 19% (FLEXPART) and 18% (LAGRANTO), and by ICT from the North American planetary boundary layer during 13% (FLEXPART) and 12% (LAGRANTO) of the entire year. Through intercomparsion with measurements, our findings suggest that both FLEXPART and LAGRANTO are well capable of representing SI and ICT events if they last for more than 12 h, whereas both have problems on representing short events. It is also shown that although the long-range transported air is characterized by relatively low NOy/CO ratios and elevated CO concentrations, using a combination of NOy/CO and CO as control parameters still encounters difficulty in distinguishing aged air masses by their source regions. Moreover, a sensitivity study indicates that the agreement between models and measurements depends significantly on the threshold values applied to the individual control parameters. Generally, the less strict the thresholds are, the better the agreement between models and measurements. Although the dependence of the agreement on the threshold values is appreciable, it nevertheless confirms the conclusion that both FLEXPART and LAGRANTO are well able to capture SI and ICT events with sustaining time longer than 12 h.


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