Regional Scale Transport Model of Atmospheric Acid Compounds, and Its Application for Hungary

Author(s):  
Katalin E. Fekete
2021 ◽  
Author(s):  
Pedro Jiménez-Guerrero ◽  
Nuno Ratola

AbstractThe atmospheric concentration of persistent organic pollutants (and of polycyclic aromatic hydrocarbons, PAHs, in particular) is closely related to climate change and climatic fluctuations, which are likely to influence contaminant’s transport pathways and transfer processes. Predicting how climate variability alters PAHs concentrations in the atmosphere still poses an exceptional challenge. In this sense, the main objective of this contribution is to assess the relationship between the North Atlantic Oscillation (NAO) index and the mean concentration of benzo[a]pyrene (BaP, the most studied PAH congener) in a domain covering Europe, with an emphasis on the effect of regional-scale processes. A numerical simulation for a present climate period of 30 years was performed using a regional chemistry transport model with a 25 km spatial resolution (horizontal), higher than those commonly applied. The results show an important seasonal behaviour, with a remarkable spatial pattern of difference between the north and the south of the domain. In winter, higher BaP ground levels are found during the NAO+ phase for the Mediterranean basin, while the spatial pattern of this feature (higher BaP levels during NAO+ phases) moves northwards in summer. These results show deviations up to and sometimes over 100% in the BaP mean concentrations, but statistically significant signals (p<0.1) of lower changes (20–40% variations in the signal) are found for the north of the domain in winter and for the south in summer.


2015 ◽  
Vol 15 (19) ◽  
pp. 10983-10998 ◽  
Author(s):  
J. C. Péré ◽  
B. Bessagnet ◽  
V. Pont ◽  
M. Mallet ◽  
F. Minvielle

Abstract. In this work, impact of aerosol solar extinction on the photochemistry over eastern Europe during the 2010 wildfires episode is discussed for the period from 5 to 12 August 2010, which coincides to the peak of fire activity. The methodology is based on an online coupling between the chemistry-transport model CHIMERE (extended by an aerosol optical module) and the radiative transfer code TUV. Results of simulations indicate an important influence of the aerosol solar extinction, in terms of intensity and spatial extent, with a reduction of the photolysis rates of NO2 and O3 up to 50 % (in daytime average) along the aerosol plume transport. At a regional scale, these changes in photolysis rates lead to a 3–15 % increase in the NO2 daytime concentration and to an ozone reduction near the surface of 1–12 %. The ozone reduction is shown to occur over the entire boundary layer, where aerosols are located. Also, the total aerosol mass concentration (PM10) is shown to be decreased by 1–2 %, on average during the studied period, caused by a reduced formation of secondary aerosols such as sulfates and secondary organics (4–10 %) when aerosol impact on photolysis rates is included. In terms of model performance, comparisons of simulations with air quality measurements at Moscow indicate that an explicit representation of aerosols interaction with photolysis rates tend to improve the estimation of the near-surface concentration of ozone and nitrogen dioxide as well as the formation of inorganic aerosol species such as ammonium, nitrates and sulfates.


Author(s):  
Jason Welsh ◽  
Jack Fishman

We use a regional scale photochemical transport model to investigate the surface concentrations and column integrated amounts of ozone (O3) and nitrogen dioxide (NO2) during a pollution event that occurred in the St. Louis metropolitan region in 2012. These trace gases will be two of the primary constituents that will be measured by TEMPO, an instrument on a geostationary platform, which will result in a dataset that has hourly temporal resolution during the daytime and ~4 km spatial resolution. Although air quality managers are most concerned with surface concentrations, satellite measurements provide a quantity that reflects a column amount, which may or may not be directly relatable to what is measured at the surface. The model results provide good agreement with observed surface O3 concentrations, which is the only trace gas dataset that can be used for verification. The model shows that a plume of O3 extends downwind from St. Louis and contains an integrated amount of ozone of ~ 16 DU (1 DU = 2.69 x 1016 mol. cm-2), a quantity that is two to three times lower than what was observed by satellite measurements during two massive pollution episodes in the 1980s. Based on the smaller isolatable emissions coming from St. Louis, this quantity is not unreasonable, but may also reflect the reduction of photochemical ozone production due to the implementation of emission controls that have gone into effect in the past few decades.


2009 ◽  
Vol 9 (14) ◽  
pp. 5281-5297 ◽  
Author(s):  
I. Pison ◽  
P. Bousquet ◽  
F. Chevallier ◽  
S. Szopa ◽  
D. Hauglustaine

Abstract. In order to study the spatial and temporal variations of the emissions of greenhouse gases and of their precursors, we developed a data assimilation system and applied it to infer emissions of CH4, CO and H2 for one year. It is based on an atmospheric chemical transport model and on a simplified scheme for the oxidation chain of hydrocarbons, including methane, formaldehyde, carbon monoxide and molecular hydrogen together with methyl chloroform. The methodology is exposed and a first attempt at evaluating the inverted fluxes is made. Inversions of the emission fluxes of CO, CH4 and H2 and concentrations of HCHO and OH were performed for the year 2004, using surface concentration measurements of CO, CH4, H2 and CH3CCl3 as constraints. Independent data from ship and aircraft measurements and satellite retrievals are used to evaluate the results. The total emitted mass of CO is 30% higher after the inversion, due to increased fluxes by up to 35% in the Northern Hemisphere. The spatial distribution of emissions of CH4 is modified by a decrease of fluxes in boreal areas up to 60%. The comparison between mono- and multi-species inversions shows that the results are close at a global scale but may significantly differ at a regional scale because of the interactions between the various tracers during the inversion.


2009 ◽  
Vol 13 (1) ◽  
pp. 69-77 ◽  
Author(s):  
E. Kalbus ◽  
C. Schmidt ◽  
J. W. Molson ◽  
F. Reinstorf ◽  
M. Schirmer

Abstract. The spatial distribution of groundwater fluxes through a streambed can be highly variable, most often resulting from a heterogeneous distribution of aquifer and streambed permeabilities along the flow pathways. Using a groundwater flow and heat transport model, we defined four scenarios of aquifer and streambed permeability distributions to simulate and assess the impact of subsurface heterogeneity on the distribution of groundwater fluxes through the streambed: (a) a homogeneous low-K streambed within a heterogeneous aquifer; (b) a heterogeneous streambed within a homogeneous aquifer; (c) a well connected heterogeneous low-K streambed within a heterogeneous aquifer; and (d) a poorly connected heterogeneous low-K streambed within a heterogeneous aquifer. The simulation results were compared with a base case scenario, in which the streambed had the same properties as the aquifer, and with observed data. The results indicated that the aquifer has a stronger influence on the distribution of groundwater fluxes through the streambed than the streambed itself. However, a homogeneous low-K streambed, a case often implemented in regional-scale groundwater flow models, resulted in a strong homogenization of fluxes, which may have important implications for the estimation of peak mass flows. The flux distributions simulated with heterogeneous low-K streambeds were similar to the flux distributions of the base case scenario, despite the lower permeability. The representation of heterogeneous distributions of aquifer and streambed properties in the model has been proven to be beneficial for the accuracy of flow simulations.


2018 ◽  
Author(s):  
Lucas Bastien ◽  
Nancy Brown ◽  
Robert Harley

Abstract. Reducing ambient formaldehyde concentrations is a complex task because formaldehyde is both a primary and a secondary air pollutant, with significant anthropogenic and biogenic sources of volatile organic compounds (VOC) precursor emissions. This work uses adjoint sensitivity analysis in a chemical transport model to identify emission sources and chemical reactions that influence formaldehyde mixing ratios in the San Francisco Bay Area, and within three urbanized sub-areas. For each of these receptors, the use of the adjoint technique allows for efficient calculation of the sensitivity of formaldehyde to emissions of NOx, formaldehyde, and VOC precursors occurring at any location and time. Formaldehyde mixing ratios are found to be generally higher in summer than in winter. The opposite seasonal trend is observed for the sensitivities of these mixing ratios to formaldehyde emissions. In other words, even though formaldehyde is higher in summer, reducing formaldehyde emissions has a greater impact in winter. In winter, 85–90 % of the sensitivity to emissions is attributed to direct formaldehyde emissions. In summer, this contribution is smaller and more variable, ranging from 26 to 72 % among the receptor areas investigated in this study. Higher relative contributions of secondary formation versus direct emissions are associated with receptors located farther away from heavily urbanized and emission-rich areas. In particular, the relative contribution of biogenic VOC emissions (15–41 % in summer) is largest for these receptors. Ethene and other alkenes are the most influential anthropogenic precursors to secondary formaldehyde. Isoprene is the most influential biogenic precursor. Sensitivities of formaldehyde to NOx emissions are generally negative, but small in magnitude compared to sensitivities to VOC emissions. The magnitude of anthropogenic emissions of organic compounds other than formaldehyde is found to correlate reasonably well with their influence on population-weighted formaldehyde mixing ratios at the air basin scale. This correlation does not hold for ambient formaldehyde in smaller urbanized sub-areas. The magnitude of biogenic emissions does not correlate with their influence in either case.


2019 ◽  
Author(s):  
Jinwoong Kim ◽  
Saroja Polavarapu ◽  
Douglas Chan ◽  
Michael Neish

Abstract. In this study, we present the development of a regional atmospheric transport model for greenhouse gas (GHG) simulation based on an operational weather forecast model and a chemical transport model at Environment and Climate Change Canada (ECCC), with the goal of improving our understanding of the high spatio-temporal resolution interaction between the atmosphere and surface GHG fluxes over Canada and the United States. The regional model uses 10 km × 10 km horizontal grid spacing and 80 vertical levels spanning the ground to 0.1 hPa. The lateral boundary conditions of meteorology and tracers are provided by the global transport model used for GHG simulation at ECCC. The performance of the regional model and added benefit of the regional model over our lower resolution global models is investigated in terms of modelled CO2 concentration and meteorological forecast quality for multiple seasons in 2015. We find that our regional model has the capability to simulate high spatial (horizontal and vertical) and temporal scales of atmospheric CO2 concentrations, based on comparisons to surface and aircraft observations. In addition, reduced bias and standard deviation of forecast error in boreal summer are obtained by the regional model. Better representation of model topography in the regional model reduces transport and representation errors significantly compared to the global model, especially in regions of complex topography, as revealed by the more precise and detailed structure of the CO2 diurnal cycle produced at observation sites and in model space. The new regional model will form the basis of a flux inversion system that estimates regional scale fluxes of GHGs over Canada.


2020 ◽  
Vol 13 (1) ◽  
pp. 269-295
Author(s):  
Jinwoong Kim ◽  
Saroja M. Polavarapu ◽  
Douglas Chan ◽  
Michael Neish

Abstract. In this study, we present the development of a regional atmospheric transport model for greenhouse gas (GHG) simulation based on an operational weather forecast model and a chemical transport model at Environment and Climate Change Canada (ECCC), with the goal of improving our understanding of the high-spatiotemporal-resolution interaction between the atmosphere and surface GHG fluxes over Canada and the United States. The regional model uses 10 km×10 km horizontal grid spacing and 80 vertical levels spanning the ground to 0.1 hPa. The lateral boundary conditions of meteorology and tracers are provided by the global transport model used for GHG simulation at ECCC. The performance of the regional model and added benefit of the regional model over our lower-resolution global models is investigated in terms of modelled CO2 concentration and meteorological forecast quality for multiple seasons in 2015. We find that our regional model has the capability to simulate the high spatial (horizontal and vertical) and temporal scales of atmospheric CO2 concentrations based on comparisons to surface and aircraft observations. In addition, the bias and standard deviation of forecast error in boreal summer are reduced by the regional model. Better representation of model topography in the regional model results in improved simulation of the CO2 diurnal cycle compared to the global model at Walnut Grove, California. The new regional model will form the basis of a flux inversion system that estimates regional-scale fluxes of GHGs over Canada.


2015 ◽  
Vol 8 (4) ◽  
pp. 3593-3651 ◽  
Author(s):  
J. Guth ◽  
B. Josse ◽  
V. Marécal ◽  
M. Joly

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.


2011 ◽  
Vol 11 (14) ◽  
pp. 7185-7207 ◽  
Author(s):  
C. Schmechtig ◽  
B. Marticorena ◽  
B. Chatenet ◽  
G. Bergametti ◽  
J. L. Rajot ◽  
...  

Abstract. The chemistry and transport model CHIMERE-DUST have been used to simulate the mineral dust cycle over the Sahara in 2006. Surface measurements deployed during the AMMA field campaign allow to test the capability of the model to correctly reproduce the atmospheric dust load and surface concentrations from the daily to the seasonal time-scale. The simulated monthly mean Aerosol Optical Depths (AOD) and surface concentrations are significantly correlated with the measured ones. The simulated daily concentrations and hourly AOD are in the same range of magnitude than the observed ones despite relatively high simulated dust emissions. The level of agreement between the simulations and the observations has been quantified at different time scales using statistical parameters classically used to evaluate air quality models. The capability of the model to reproduce the altitude of the dust transport was tested for two contrasted cases of low and high altitude transport. These results highlight the sensitivity of the simulations to the surface winds used as external forcing and the necessity to further constrain the dust mass budget at the regional scale.


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