scholarly journals Response of secondary inorganic aerosol concentrations and deposition fluxes of S and N across Germany to emission changes during high PM<sub>10</sub> episodes in spring 2009

2013 ◽  
Vol 13 (6) ◽  
pp. 15783-15827 ◽  
Author(s):  
S. Banzhaf ◽  
M. Schaap ◽  
R. J. Wichink Kruit ◽  
H. A. C. Denier van der Gon ◽  
R. Stern ◽  
...  
Keyword(s):  
Western Europe ◽  
Transport Model ◽  
N Deposition ◽  
Chemistry Transport Model ◽  
Deposition Fluxes ◽  
Nh3 Emission ◽  
Non Linear ◽  
Inorganic Aerosol ◽  
Emission Changes ◽  
North Western

Abstract. In this study, the response of secondary inorganic aerosol (SIA) concentrations to changes in precursor emissions during high PM10 episodes over Central Europe in spring 2009 was investigated with the Eulerian Chemistry Transport Model (CTM) REM-Calgrid (RCG). The model performed well in capturing the temporal variation of PM10 and SIA concentrations and was used to analyse the different origin, development and characteristics of the selected high PM10 episodes. SIA concentrations, which attribute to about 50% of the PM10 concentration in north-western Europe, have been studied by means of several emission scenarios varying SO2, NOx and NH3 emissions within a domain covering Germany and within a domain covering Europe. It was confirmed that the response of sulphate, nitrate and ammonium concentrations and deposition fluxes of S and N to SO2, NOx and NH3 emission changes is non-linear. The deviation from linearity was found to be lower for total deposition fluxes of S and N than for SIA concentrations. Furthermore, the study has shown that incorporating explicit cloud chemistry in the model adds non-linear responses to the system and significantly modifies the response of modelled SIA concentrations and S and N deposition fluxes to changes in precursor emissions. The analysis of emission reduction scenarios demonstrates that next to European wide emission reductions additional national NH3 measures in Germany are more effective in reducing SIA concentrations and deposition fluxes than additional national measures on SO2 and NOx.

scholarly journals Impact of emission changes on secondary inorganic aerosol episodes across Germany

2013 ◽  
Vol 13 (23) ◽  
pp. 11675-11693 ◽  
Author(s):  
S. Banzhaf ◽  
M. Schaap ◽  
R. J. Wichink Kruit ◽  
H. A. C. Denier van der Gon ◽  
R. Stern ◽  
...  
Keyword(s):  
Transport Model ◽  
N Deposition ◽  
Emission Scenarios ◽  
Cloud Chemistry ◽  
Chemistry Transport Model ◽  
Deposition Fluxes ◽  
Nh3 Emission ◽  
Non Linear ◽  
Inorganic Aerosol ◽  
Emission Changes

Abstract. In this study, the response of secondary inorganic aerosol (SIA) concentrations to changes in precursor emissions during high PM10 episodes over central Europe in spring 2009 was investigated with the Eulerian Chemistry Transport Model (CTM) REM-Calgrid (RCG). The model performed well in capturing the temporal variation of PM10 and SIA concentrations and was used to analyse the different origin, development and characteristics of the selected high PM10 episodes. SIA concentrations, which contribute to about 50% of the PM10 concentration in northwestern Europe, have been studied by means of several model runs for different emission scenarios. SO2, NOx and NH3 emissions have been varied within a domain covering Germany and within a domain covering Europe. It was confirmed that the response of sulfate, nitrate and ammonium concentrations and deposition fluxes of S and N to SO2, NOx and NH3 emission changes is non-linear. The deviation from linearity was found to be lower for total deposition fluxes of S and N than for SIA concentrations. Furthermore, the study has shown that incorporating explicit cloud chemistry in the model adds non-linear responses to the system. It significantly modifies the response of modelled SIA concentrations and S and N deposition fluxes to changes in precursor emissions. The analysis of emission reduction scenario runs demonstrates that next to European-wide emission reductions additional national NH3 measures in Germany are more effective in reducing SIA concentrations and deposition fluxes than additional national measures on SO2 and NOx.

scholarly journals Dynamic model evaluation for secondary inorganic aerosol and its precursors over Europe between 1990 and 2009

2015 ◽  
Vol 8 (4) ◽  
pp. 1047-1070 ◽  
Author(s):  
S. Banzhaf ◽  
M. Schaap ◽  
R. Kranenburg ◽  
A. M. M. Manders ◽  
A. J. Segers ◽  
...  
Keyword(s):  
Nitrogen Dioxide ◽  
Interannual Variability ◽  
Dynamic Model ◽  
Model Evaluation ◽  
Climate Model ◽  
Transport Model ◽  
Non Linear ◽  
Concentration Changes ◽  
Inorganic Aerosol ◽  
Emission Changes

Abstract. In this study we present a dynamic model evaluation of chemistry transport model LOTOS-EUROS (LOng Term Ozone Simulation – EURopean Operational Smog) to analyse the ability of the model to reproduce observed non-linear responses to emission changes and interannual variability of secondary inorganic aerosol (SIA) and its precursors over Europe from 1990 to 2009. The 20 year simulation was performed using a consistent set of meteorological data provided by RACMO2 (Regional Atmospheric Climate MOdel). Observations at European rural background sites have been used as a reference for the model evaluation. To ensure the consistency of the used observational data, stringent selection criteria were applied, including a comprehensive visual screening to remove suspicious data from the analysis. The LOTOS-EUROS model was able to capture a large part of the seasonal and interannual variability of SIA and its precursors' concentrations. The dynamic evaluation has shown that the model is able to simulate the declining trends observed for all considered sulfur and nitrogen components following the implementation of emission abatement strategies for SIA precursors over Europe. Both the observations and the model show the largest part of the decline in the 1990s, while smaller concentration changes and an increasing number of non-significant trends are observed and modelled between 2000 and 2009. Furthermore, the results confirm former studies showing that the observed trends in sulfate and total nitrate concentrations from 1990 to 2009 are lower than the trends in precursor emissions and precursor concentrations. The model captured well these non-linear responses to the emission changes. Using the LOTOS-EUROS source apportionment module, trends in the formation efficiency of SIA have been quantified for four European regions. The exercise has revealed a 20–50% more efficient sulfate formation in 2009 compared to 1990 and an up to 20% more efficient nitrate formation per unit nitrogen oxide emission, which added to the explanation of the non-linear responses. However, we have also identified some weaknesses in the model and the input data. LOTOS-EUROS underestimates the observed nitrogen dioxide concentrations throughout the whole time period, while it overestimates the observed nitrogen dioxide concentration trends. Moreover, model results suggest that the emission information of the early 1990s used in this study needs to be improved concerning magnitude and spatial distribution.

scholarly journals Dynamic model evaluation for secondary inorganic aerosol and its precursors over Europe between 1990 and 2009

2014 ◽  
Vol 7 (4) ◽  
pp. 4645-4703 ◽  
Author(s):  
S. Banzhaf ◽  
M. Schaap ◽  
R. Kranenburg ◽  
A. M. M. Manders ◽  
A. J. Segers ◽  
...  
Keyword(s):  
Nitrogen Dioxide ◽  
Interannual Variability ◽  
Dynamic Model ◽  
Model Evaluation ◽  
Climate Model ◽  
Transport Model ◽  
Non Linear ◽  
Concentration Changes ◽  
Inorganic Aerosol ◽  
Emission Changes

Abstract. In this study we present a dynamic model evaluation of the chemistry transport model LOTOS-EUROS to analyse the ability of the model to reproduce observed non-linear responses to emission changes and interannual variability of secondary inorganic aerosol (SIA) and its precursors over Europe from 1990 to 2009. The 20 year simulation was performed using a consistent set of meteorological data provided by the regional climate model RACMO2. Observations at European rural background sites have been used as reference for the model evaluation. To ensure the consistency of the used observational data stringent selection criteria were applied including a comprehensive visual screening to remove suspicious data from the analysis. The LOTOS-EUROS model was able to capture a large part of the day-to-day, seasonal and interannual variability of SIA and its precursors' concentrations. The dynamic evaluation has shown that the model is able to simulate the declining trends observed for all considered sulphur and nitrogen components following the implementation of emission abatement strategies for SIA precursors over Europe. Both, the observations and the model show the largest part of the decline in the 1990's while smaller concentration changes and an increasing number of non-significant trends are observed and modelled between 2000–2009. Furthermore, the results confirm former studies showing that the observed trends in sulphate and total nitrate concentrations from 1990 to 2009 are significantly lower than the trends in precursor emissions and precursor concentrations. The model captured these non-linear responses to the emission changes well. Using the LOTOS-EUROS source apportionment module trends in formation efficiency of SIA have been quantified for four European regions. The exercise has revealed a 20–50% more efficient sulphate formation in 2009 compared to 1990 and an up to 20% more efficient nitrate formation per unit nitrogen oxide emission, which added to the explanation of the non-linear responses. However, we have also identified some weaknesses to the model and the input data. LOTOS-EUROS underestimates the observed nitrogen dioxide concentrations throughout the whole time period, while it overestimates the observed nitrogen dioxide concentration trends. Moreover, model results suggest that the emission information of the early 1990's used in this study needs to be improved concerning magnitude and spatial distribution.

scholarly journals Simulating Secondary Inorganic Aerosols using the chemistry transport model MOCAGE version R2.15.0

2015 ◽  
Vol 8 (4) ◽  
pp. 3593-3651 ◽  
Author(s):  
J. Guth ◽  
B. Josse ◽  
V. Marécal ◽  
M. Joly
Keyword(s):  
North America ◽  
Transport Model ◽  
Regional Scale ◽  
In Situ Measurements ◽  
Aerosol Composition ◽  
Chemistry Transport Model ◽  
Inorganic Aerosols ◽  
Modis Aod ◽  
Inorganic Aerosol

Abstract. In this study we develop a Secondary Inorganic Aerosol (SIA) module for the chemistry transport model MOCAGE developed at CNRM. Based on the thermodynamic equilibrium module ISORROPIA II, the new version of the model is evaluated both at the global scale and at the regional scale. The results show high concentrations of secondary inorganic aerosols in the most polluted regions being Europe, Asia and the eastern part of North America. Asia shows higher sulfate concentrations than other regions thanks to emissions reduction in Europe and North America. Using two simulations, one with and the other without secondary inorganic aerosol formation, the model global outputs are compared to previous studies, to MODIS AOD retrievals, and also to in situ measurements from the HTAP database. The model shows a better agreement in all geographical regions with MODIS AOD retrievals when introducing SIA. It also provides a good statistical agreement with in situ measurements of secondary inorganic aerosol composition: sulfate, nitrate and ammonium. In addition, the simulation with SIA gives generally a better agreement for secondary inorganic aerosols precursors (nitric acid, sulfur dioxide, ammonia) in particular with a reduction of the Modified Normalised Mean Bias (MNMB). At the regional scale, over Europe, the model simulation with SIA are compared to the in situ measurements from the EMEP database and shows a good agreement with secondary inorganic aerosol composition. The results at the regional scale are consistent with those obtained with the global simulations. The AIRBASE database was used to compare the model to regulated air quality pollutants being particulate matter, ozone and nitrogen dioxide concentrations. The introduction of the SIA in MOCAGE provides a reduction of the PM2.5 MNMB of 0.44 on a yearly basis and even 0.52 on a three spring months period (March, April, May) when SIA are maximum.

Variability of PM pollution in the light of emission changes and meteorological variability: a case study for Styria, Austria

2020 ◽  
Author(s):  
Christian A. Schmidt ◽  
Peter Huszár ◽  
Monika Mayer ◽  
Johannes Fritzer ◽  
Harald E. Rieder
Keyword(s):  
Air Pollution ◽  
Emission Reduction ◽  
Transport Model ◽  
Special Importance ◽  
Chemistry Transport Model ◽  
The Alps ◽  
Industrial Regions ◽  
Emission Changes ◽  
Local Emissions

&lt;p&gt;Despite ambitious efforts to abate surface air pollution, the air quality thresholds for PM10 and PM2.5 are regularly exceeded in the state of Styria. PM target levels are most frequently exceeded in industrial regions and urban cores of the forelands preceeding the alps. Besides local emissions, ambient meteorology and particularly stagnation are of special importance for PM pollution. Here we assess local and regional changes in PM pollution following emission reduction measures, while simultaneously considering effects of meteorological variability. We further supplement our observational study with a set of high-resolution chemistry-transport-model (CTM) simulations to assess future changes in the PM burden in Styria.&lt;/p&gt;

scholarly journals Interannual variability of tropospheric composition: the influence of changes in emissions, meteorology and clouds

2010 ◽  
Vol 10 (5) ◽  
pp. 2491-2506 ◽  
Author(s):  
A. Voulgarakis ◽  
N. H. Savage ◽  
O. Wild ◽  
P. Braesicke ◽  
P. J. Young ◽  
...  
Keyword(s):  
Interannual Variability ◽  
Biomass Burning ◽  
Strong Influence ◽  
Transport Model ◽  
Global Scale ◽  
Meteorological Conditions ◽  
Shortwave Radiation ◽  
Chemistry Transport Model ◽  
Attribution Analysis ◽  
Emission Changes

Abstract. We have run a chemistry transport model (CTM) to systematically examine the drivers of interannual variability of tropospheric composition during 1996–2000. This period was characterised by anomalous meteorological conditions associated with the strong El Niño of 1997–1998 and intense wildfires, which produced a large amount of pollution. On a global scale, changing meteorology (winds, temperatures, humidity and clouds) is found to be the most important factor driving interannual variability of NO2 and ozone on the timescales considered. Changes in stratosphere-troposphere exchange, which are largely driven by meteorological variability, are found to play a particularly important role in driving ozone changes. The strong influence of emissions on NO2 and ozone interannual variability is largely confined to areas where intense biomass burning events occur. For CO, interannual variability is almost solely driven by emission changes, while for OH meteorology dominates, with the radiative influence of clouds being a very strong contributor. Through a simple attribution analysis for 1996–2000 we conclude that changing cloudiness drives 25% of the interannual variability of OH over Europe by affecting shortwave radiation. Over Indonesia this figure is as high as 71%. Changes in cloudiness contribute a small but non-negligible amount (up to 6%) to the interannual variability of ozone over Europe and Indonesia. This suggests that future assessments of trends in tropospheric oxidizing capacity should account for interannual variability in cloudiness, a factor neglected in many previous studies.

scholarly journals Impacts of climate and emission changes on nitrogen deposition in Europe: a multi-model study

2014 ◽  
Vol 14 (5) ◽  
pp. 6663-6720 ◽  
Author(s):  
D. Simpson ◽  
C. Andersson ◽  
J.H. Christensen ◽  
M. Engardt ◽  
C. Geels ◽  
...  
Keyword(s):  
Critical Loads ◽  
N Deposition ◽  
Scale Model ◽  
Gaseous Ammonia ◽  
Nh3 Emission ◽  
Model Study ◽  
Emission Changes ◽  
Emission Change ◽  
The Impact ◽  
Oxidised Nitrogen

Abstract. The impact of climate and emissions changes on the deposition of reactive nitrogen (Nr) over Europe was studied using four offline regional chemistry transport models (CTMs) driven by the same global projection of future climate over the period 2000–2050. Anthropogenic emissions for the years 2005 and 2050 were used for simulations of both present and future periods in order to isolate the impact of climate change, hemispheric boundary conditions and emissions, and to assess the robustness of the result across the different models. The results from these four CTMs clearly show that the main driver of future N-deposition changes is the specified emission change. Under the specified emission scenario for 2050, emissions of oxidised nitrogen were reduced substantially, whereas emissions of NH3 increase to some extent, and these changes are largely reflected in the modelled concentrations and depositions. The lack of sulphur and oxidised nitrogen in the future atmosphere results in a much larger fraction of NHx being present in the form of gaseous ammonia. Predictions for wet and total deposition were broadly consistent, although the three fine-scale models resolve European emission areas and changes better than the hemispheric-scale model. The biggest difference in the models is for predictions of individual N-compounds. One model (EMEP) was used to explore changes in critical loads, also in conjunction with speculative climate-induced increases in NH3 emissions. These calculations suggest that the area of ecosystems which exceed critical loads is reduced from 64% for year 2005 emissions levels to 50% for currently estimated 2050 levels. A possible climate-induced increase in NH3 emissions could worsen the situation, with areas exceeded increasing again to 57% (for a 30% NH3 emission increase).

scholarly journals Modelling the mineralogical composition and solubility of mineral dust in the Mediterranean area with CHIMERE 2017r4

2020 ◽  
Vol 13 (4) ◽  
pp. 2051-2071 ◽  
Author(s):  
Laurent Menut ◽  
Guillaume Siour ◽  
Bertrand Bessagnet ◽  
Florian Couvidat ◽  
Emilie Journet ◽  
...  
Keyword(s):  
Optical Properties ◽  
Transport Model ◽  
Mineral Dust ◽  
Mineralogical Composition ◽  
Mediterranean Area ◽  
Mineral Species ◽  
Chemistry Transport Model ◽  
Deposition Fluxes ◽  
Global Databases ◽  
Radiative Impact

Abstract. Modelling of mineral dust is often done using one single mean species. But for biogeochemical studies, it could be useful to access to a more detailed information on differentiated mineral species and the associated chemical composition. Differentiating between mineral species would also induce different optical properties and densities and then different radiative impact, transport and deposition. In this study, the mineralogical differentiation is implemented in the CHIMERE regional chemistry-transport model, by using global databases. The results show that this implementation does not change the results much in terms of aerosol optical depth, surface concentrations and deposition fluxes. But the information on mineralogy, with a high spatial (a few kilometres) and temporal (1 h) resolution, is now available and is ready to be used for future biogeochemical studies.

scholarly journals Dry and wet deposition of inorganic nitrogen compounds to a tropical pasture site (Rondônia, Brazil)

2006 ◽  
Vol 6 (2) ◽  
pp. 447-469 ◽  
Author(s):  
I. Trebs ◽  
L. L. Lara ◽  
L. M. M. Zeri ◽  
L. V. Gatti ◽  
P. Artaxo ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Dry Deposition ◽  
Wet Deposition ◽  
Particle Deposition ◽  
Inorganic Nitrogen ◽  
N Deposition ◽  
Deposition Fluxes ◽  
Dry And Wet Deposition ◽  
Surface Atmosphere ◽  
Nh3 Emission

Abstract. The input of nitrogen (N) to ecosystems has increased dramatically over the past decades. While total (wet + dry) N deposition has been extensively determined in temperate regions, only very few data sets of N wet deposition exist for tropical ecosystems, and moreover, reliable experimental information about N dry deposition in tropical environments is lacking. In this study we estimate dry and wet deposition of inorganic N for a remote pasture site in the Amazon Basin based on in-situ measurements. The measurements covered the late dry (biomass burning) season, a transition period and the onset of the wet season (clean conditions) (12 September to 14 November 2002) and were a part of the LBA-SMOCC (Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall, and Climate) 2002 campaign. Ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), nitrogen dioxide (NO2), nitric oxide (NO), ozone (O3), aerosol ammonium (NH4+) and aerosol nitrate (NO3-) were measured in real-time, accompanied by simultaneous meteorological measurements. Dry deposition fluxes of NO2 and HNO3 are inferred using the ''big leaf multiple resistance approach'' and particle deposition fluxes are derived using an established empirical parameterization. Bi-directional surface-atmosphere exchange fluxes of NH3 and HONO are estimated by applying a ''canopy compensation point model''. N dry and wet deposition is dominated by NH3 and NH4+, which is largely the consequence of biomass burning during the dry season. The grass surface appeared to have a strong potential for daytime NH3 emission, owing to high canopy compensation points, which are related to high surface temperatures and to direct NH3 emissions from cattle excreta. NO2 also significantly accounted for N dry deposition, whereas HNO3, HONO and N-containing aerosol species were only minor contributors. Ignoring NH3 emission from the vegetation surface, the annual net N deposition rate is estimated to be about −11 kgN ha-1 yr-1. If on the other hand, surface-atmosphere exchange of NH3 is considered to be bi-directional, the annual net N budget at the pasture site is estimated to range from −2.15 to −4.25 kgN ha-1 yr-1.

scholarly journals Nitrogen deposition in the UK at 1 km resolution from 1990 to 2017

2021 ◽  
Author(s):  
Samuel James Tomlinson ◽  
Edward John Carnell ◽  
Anthony J. Dore ◽  
Ulrike Dragosits
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
N Deposition ◽  
Nitrogen Oxide Emissions ◽  
Chemistry Transport Model ◽  
Wet And Dry Deposition ◽  
Coarse Spatial Resolution ◽  
Reduce Emissions ◽  
The Uk

Abstract. An atmospheric chemistry transport model (FRAME) is used here to calculate the UK N deposition for the years 1990–2017. Reactive nitrogen (N) deposition is a threat that can lead to adverse effects on the environment and human health. In Europe, substantial reductions in N deposition from nitrogen oxide emissions have been achieved in recent decades, this paper quantifies reductions in UK N deposition following the N emissions peak in 1990. In the UK, estimates of N deposition are typically available at a coarse spatial resolution (typically 5 km × 5 km grid resolution) and it is often difficult to compare estimates between years due to methodological changes in emission estimates. Through efforts to reduce emissions of N from industry, traffic, and agriculture, this study predicts that UK N deposition has reduced from 465 kt N in 1990 to 278 kt N in 2017. However, as part of this overall reduction, there are non-uniform changes for wet and dry deposition of reduced N (NHx) and oxidised N (NOy). In 2017, it is estimated 59 % of all N deposition is in the form of reduced N, a change from 35 % in 1990. This dataset uses 28 years of emissions data from 1990 to 2017 to produce the first long-term dataset of 28 years of N deposition at 1 km × 1 km resolution in the UK.

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